Self-feedback intelligent electrochemical wastewater treatment platform and construction method thereof

Abstract

The invention discloses a self-feedback intelligent electrochemical wastewater treatment platform and a construction method thereof. The platform modularly integrates an electrochemical water treatment unit, a terephthalic acid probe molecular fluorescence sensing unit, a signal acquisition data processing unit and an electro-hydraulic linkage online control unit. All the units work cooperatively, and the electrochemical water treatment unit generates strong oxidizing hydroxyl radical mineralized pollutants; the fluorescence sensing and data processing unit is used for converting. OH specificity into a fluorescence signal by utilizing probe molecules and mapping the fluorescence signal into. OH steady-state equivalent concentration in real time; and the online control unit implements a model prediction control strategy based on concentration feedback, dynamically adjusts the current density, the electrode potential and the wastewater flow, and realizes real-time adaptive matching of the interface mass transfer and the. OH generation rate. According to the invention, electrogenerated. OH on-line monitoring and dynamic closed-loop optimization of operation parameters are realized, deep mineralization, low energy consumption and long-term stable operation are realized, and the method is suitable for engineering and intelligent operation of electrochemical advanced oxidation treatment of industrial wastewater.

Description

Technical Field

[0001] This invention relates to the field of water pollution control and electrochemical advanced oxidation technology, and more specifically, to a self-feedback intelligent electrochemical wastewater treatment platform and its construction method. Background Technology

[0002] With the acceleration of industrialization and urbanization, wastewater discharged from industries such as pharmaceuticals, printing and dyeing, and chemicals contains a variety of recalcitrant organic pollutants. These pollutants are difficult to completely remove using conventional biological treatment methods, seriously threatening the ecological environment and water resource security. Traditional wastewater treatment technologies have significant shortcomings in terms of treatment efficiency, energy consumption, and adaptability to complex water qualities, making it difficult to meet the needs of in-depth industrial wastewater treatment.

[0003] In recent years, electrochemical advanced oxidation (EAO) has provided a green and controllable deep treatment pathway for wastewater by directly activating molecular oxygen or water at the electrode interface to generate highly reactive oxygen species such as hydroxyl radicals (·OH). However, in actual engineering operation, it faces systemic bottlenecks: (1) Mass transfer is limited: the solubility and diffusion rate of dissolved oxygen in the water body are low, and the concentration of pollutants in the reaction zone decreases along the way, resulting in the attenuation of the interfacial concentration gradient and mass transfer driving force, making it difficult to maintain a working state close to the limiting current density; (2) Mismatch between constant parameter operation and operating condition changes: open-loop operation modes such as constant current or constant potential cannot synchronously adjust the electrolysis conditions with changes in influent water quality, flow rate and temperature, the ·OH generation rate is prone to fluctuation, and side reactions (such as excessive oxygen evolution or by-product generation) are triggered, causing an increase in energy consumption; (3) Lack of process characterization and online quantification for ·OH generation: most engineering scenarios only monitor conventional water quality indicators, and lack rapid and interference-resistant quantification methods for key intermediate processes (such as the effective supply and utilization of ·OH), making it difficult to support device-level optimization and long-term steady-state operation.

[0004] Therefore, there is an urgent need for an electrochemical wastewater treatment platform that can sense key reaction characteristics online and adjust electrolysis parameters and hydraulic conditions accordingly, so as to achieve dynamic matching of interfacial mass transfer and reaction rate, reduce energy consumption and suppress operational fluctuations, and adapt to the long-term continuous operation requirements under complex and fluctuating water quality. Summary of the Invention

[0005] The purpose of this invention is to propose a self-feedback intelligent electrochemical wastewater treatment platform and its construction method, aiming to solve the following technical problems: the attenuation of interfacial mass transfer driving force caused by pollutant mineralization along the process, the mismatch between current efficiency and mass transfer under constant electrolysis conditions, and the resulting fluctuations in ·OH generation and increased energy consumption due to side reactions, among other engineering challenges. Through real-time monitoring and predictive closed-loop control, this invention aims to achieve adaptive matching between electrolysis parameters and the interfacial mass transfer-reaction process, thereby maintaining efficient, low-consumption, and stable operation under complex water quality conditions.

[0006] To achieve the above objectives, the present invention proposes the following technical solution:

[0007] A self-feedback intelligent electrochemical wastewater treatment platform and its construction method, the construction method comprising the following steps:

[0008] S1 Reactor and Electrode Construction: Set up an electrocatalytic anode and cathode that can generate hydroxyl radicals, configure a reference electrode, a programmable power supply, a programmable peristaltic pump or flow control device, and an electrode surface sampling port;

[0009] S2 terephthalic acid probe molecule capture configuration: Prepare an acidic buffer solution with pH 3.5-4.5 and a 0.1-1 mM TA capture solution to capture electrogenerated hydroxyl radicals on the surface of the electrocatalytic active electrode and generate the specific hydroxylated fluorescent product HTA;

[0010] S3 Optical Module Installation and Calibration: Establish a mapping model between fluorescence intensity and equivalent concentration of hydroxyl radicals in a constant temperature dark chamber, and store the calibration parameters in the controller;

[0011] S4 Online Sampling and In-situ Fluorescence Detection: Fluorescence signals are periodically acquired via a bypass microfluidic channel or a patch-type sensing unit. The reaction microregion contains a TA (transferase) and an inert fluorescent reference material, coated with a hydrophobic barrier membrane. The bypass channel flow rate is 0.2 to 1.0 mL / min. -1 ;

[0012] S5 Algorithm Solution and Closed-Loop Control: Real-time calculation of the equivalent concentration of hydroxyl radicals, estimation of interfacial mass transfer capacity based on the limiting current model and formation of constraints, and adjustment of electrolysis parameters through model predictive control algorithm to achieve self-feedback closed-loop control;

[0013] S6 Anti-interference and self-cleaning: The reference channel or internal reference is proportionalized to perform background subtraction and drift compensation, and acid washing / backwashing and optical and temperature self-checks are performed periodically;

[0014] S7 Long-Term Drift Calibration: Perform two-point calibration daily or weekly;

[0015] The steps are performed in parallel in the order described to build and run the intelligent platform.

[0016] This invention further provides an intelligent platform constructed using the above-described construction method:

[0017] Furthermore, the intelligent platform modularly integrates an electrochemical water treatment unit, a terephthalic acid probe molecule fluorescence sensing unit, a signal acquisition and data processing unit, and an electro-hydraulic linkage online control unit; each unit communicates via Ethernet or RS-485 and achieves pluggable integration through standardized electrical and fluid interfaces; the platform is used to monitor the steady-state equivalent concentration of hydroxyl radicals online and dynamically adjust electrolysis parameters under the constraints of model predictive control algorithms, thereby achieving efficient, stable, and energy-saving operation of the electrochemical oxidation process.

[0018] The electrochemical water treatment unit is suitable for deep wastewater treatment. It generates hydroxyl radicals in situ at the electrode interface through anodic electrocatalytic oxidation, cathodic electro-Fenton, or a combination thereof, thereby achieving deep mineralization of recalcitrant organic pollutants. A bypass or in-situ microfluidic monitoring area is set in the area adjacent to the surface of the electrogenerated hydroxyl radical electrode.

[0019] Furthermore, the anode is a boron-doped diamond, titanium suboxide, Ti / SnO2, Ti / PbO2, RuO2, or IrO2-based mixed metal oxide electrode; the cathode is a gas diffusion electrode, carbon felt, graphite felt, graphene-supported electrode, or an iron-based single-atom catalyst, Fe-NC material, Fe-MOF, or iron sulfide-carbon composite material modified on its surface.

[0020] Furthermore, the terephthalic acid probe molecule fluorescence sensing unit is a bypass microfluidic channel or a patch-type gel sensing patch. The channel or patch contains a buffer system with a pH of 3.5-4.5 and a TA substrate to specifically capture hydroxyl radicals and generate the fluorescent adduct product hydroxylated terephthalic acid. The terephthalic acid probe molecule fluorescence sensing unit is coated with a hydrophobic anti-interference barrier membrane and equipped with a reference branch for background subtraction. The bypass microfluidic channel has an optical path length of 1-2 mm and a flow rate of 0.2-1.0 mL / min. -1 The response time is ≤30 s; the patch-type gel sensor uses PVA-alginate or polyacrylamide gel and encapsulates an inert fluorescent reference to achieve ratiometric self-calibration; and background subtraction, drift compensation and ratiometric algorithms are implemented at the data processing end before operation to improve the measurement accuracy of steady-state hydroxyl equivalent concentration.

[0021] Furthermore, the signal acquisition and data processing unit is communicatively connected to the terephthalic acid probe molecule fluorescence sensing unit, and is used to preprocess and quantitatively fit the fluorescence signal, map the fluorescence signal to the steady-state equivalent concentration of hydroxyl radicals, and perform matrix correction; the signal acquisition and data processing unit includes a constant illuminance ultraviolet excitation source, an emission bandpass filter element, and a photodetector, wherein the bandpass filter photodetector is a PMT, CCD, or CMOS, which acquires HTA fluorescence signals in the 425-430 nm band and is set in a dark box or integrating sphere to ensure uniform light collection.

[0022] Furthermore, the signal acquisition and data processing unit also includes a temperature and illuminance drift compensation module and a reference channel. The intelligent platform can be configured in parallel with the electrochemical detection of HTA products as a redundant signal to further improve the detection reliability of the fluorescence signal.

[0023] Furthermore, the electro-hydraulic linkage online control unit includes a programmable DC power supply, a programmable peristaltic pump or flow regulating device, a controller, and an algorithm processing module for monitoring the electrode potential, a reference electrode, and a sampling interface; data communication is performed via Ethernet or RS-485 bus, and pluggable connection is achieved through standardized electrical terminals and fluid connectors; the controller receives the output signal of the TA fluorescence sensing unit in real time, extracts the instantaneous ·OH concentration feature information through a graph neural network, and calculates and outputs closed-loop control commands based on a model predictive control algorithm.

[0024] Furthermore, the model predictive control algorithm combines real-time fluorescence sensing signals and actual electrolysis parameters to estimate interfacial mass transfer capacity with limiting current density as a constraint. It then adjusts the current density, electrode potential, and hydraulic retention time in real time, using removal rate and unit energy consumption as objective functions. This enables adaptive regulation of the interfacial hydroxyl generation rate and pollutant mineralization rate under complex water quality conditions, maintaining efficient and low-consumption stable operation.

[0025] Furthermore, the system incorporates anti-interference and self-cleaning strategies, including reference differential background subtraction, hydrophobic barrier membrane, timed chemical or acid washing self-cleaning procedures, optical and temperature self-checks, and background subtraction, drift compensation, and ratioing algorithms implemented at the data end to improve steady-state measurement accuracy.

[0026] Furthermore, to improve system applicability and industrial scalability, the present invention preferably designs each unit in a modular manner and supports parallel or series expansion to adapt to engineering scale-up of different processing capabilities and operating modes; at the same time, the controller can be configured with remote monitoring and data logging functions to implement fault diagnosis, maintenance strategy optimization and long-term optimization of operating parameters.

[0027] In summary, the present invention has the following beneficial effects:

[0028] 1. The platform obtains the steady-state equivalent concentration of hydroxyl radicals through online fluorescence sensing, and implements model predictive control closed-loop control based on the limiting current model. It dynamically optimizes operating parameters in real time, adjusts current density, electrode potential and wastewater flow rate, and achieves dynamic matching between hydroxyl generation rate and interfacial mass transfer, thereby maintaining efficient deep mineralization of pollutants under complex water quality conditions.

[0029] 2. The platform adjusts its operating parameters based on real-time monitoring signals to avoid the accumulation of side reactions caused by excessive or insufficient energy consumption under constant electrolysis, thereby significantly reducing system energy consumption and improving the safety and stability of the processing.

[0030] 3. The platform adopts a modular design to achieve unit integration, and has a built-in online self-cleaning program and long-term drift calibration mechanism, which makes the system easy to scale up in engineering, operate continuously and maintain on site, reducing operation and maintenance costs and improving availability;

[0031] 4. The platform integrates online monitoring, dynamic control and self-maintenance functions, and is suitable for continuous treatment of high-load industrial wastewater in industries such as pharmaceuticals, printing and dyeing, and chemicals. It has good engineering adaptability and industrialization potential. Attached Figure Description

[0032] Figure 1 Schematic diagram of a self-feedback intelligent platform for electrochemical oxidation wastewater treatment;

[0033] Figure 2 Operation logic diagram of the self-feedback intelligent platform for electrochemical oxidation wastewater treatment;

[0034] Figure 3 Schematic diagram of mass transfer and reaction in an electrocatalytic water treatment unit;

[0035] Figure 4 Schematic diagram of the online fluorescence sensing process for hydroxyl radicals using probe molecules;

[0036] Figure 5 Online closed-loop control logic block diagram;

[0037] Figure 6 Logic flowchart of the self-feedback intelligent platform for electrochemical oxidation wastewater treatment;

[0038] Figure 7 Platform performance comparison diagram. Detailed Implementation

[0039] The present invention will be described in detail below with reference to the accompanying drawings and embodiments, but the present invention is not limited to these embodiments.

[0040] Example 1: Construction and Operation of a High-Efficiency, Low-Electrochemical Intelligent Platform for Wastewater Treatment

[0041] The high-efficiency, low-consumption electrochemical wastewater treatment intelligent platform and construction method of this embodiment are based on the collaborative operation of an electrochemical water treatment unit, a fluorescent molecular probe sensing unit, an optical signal acquisition and data processing unit, and an electro-hydraulic linkage online control unit with established communication. Each unit achieves real-time information transmission and linkage control through a data signal interface, thereby realizing adaptive intelligent regulation of the wastewater treatment process. The intelligent platform is as follows... Figure 1 As shown, it includes:

[0042] 1. Electrochemical water treatment unit:

[0043] The electrochemical water treatment unit includes an electrolytic cell and its supporting facilities, and can employ an electrocatalytic oxidation system to achieve deep mineralization of recalcitrant organic matter in wastewater. Specific configurations include:

[0044] Wastewater samples: contain recalcitrant organic matter, chemical oxygen demand (COD) 10-1000 mg / L;

[0045] The anode can be selected from Ti4O7, BDD, RuO2 / Ti, or other inert electrodes that can generate hydroxyl radicals by electrolysis;

[0046] The cathode may be a conductive counter electrode, a gas diffusion electrode, or a Fe-based catalyst electrode modified with the electrode surface thereof;

[0047] The unit establishes data communication with other units through a controllable DC power supply and an adjustable peristaltic pump, enabling online control of current density, electrode potential, and water flow velocity.

[0048] 2. Terephthalic acid (TA) probe molecule fluorescence sensing unit:

[0049] This probe is used to capture hydroxyl radicals in real time and generate detectable fluorescent adduct products (HTAs); the probe molecules are prepared in an acidic buffer solution at pH 3.5-4.5 and placed in a bypass microfluidic channel at a flow rate of 0.2-1.0 mL / min. -1 Response time ≤ 30 s.

[0050] 3. Optical signal acquisition and data processing unit:

[0051] It includes a constant-illuminance UV excitation source (approximately 315 nm) and a bandpass filter detector (425-430 nm, PMT, CCD, or CMOS), which are installed in a dark box or integrating sphere to ensure uniform light collection. The unit maps fluorescence intensity to the steady-state equivalent concentration of hydroxyl radicals through multi-point calibration and matrix correction algorithms, and outputs the result to the controller.

[0052] 4. Electro-hydraulic linkage online control unit:

[0053] The system includes an adjustable DC power supply, a peristaltic pump or flow regulating device, a reference electrode for electrode potential monitoring, a computer controller, and control software. The controller receives fluorescence sensor signals via a dedicated data interface, extracts real-time ·OH concentration characteristics using a graph neural network, and generates closed-loop control commands based on a model predictive control algorithm using a limiting current model, thereby achieving dynamic adjustment of electrolysis parameters and hydraulic residence time.

[0054] The method for constructing the intelligent platform includes the following steps:

[0055] Reactor and Electrode Construction: The reactor is equipped with an anode (e.g., Ti4O7) and a cathode (e.g., a stainless steel conductive counter electrode), and a wastewater sampling port or patch window is provided. The controllable DC power supply is connected to a communication interface (e.g., RS485, Modbus, or Ethernet) to achieve online control of current density and electrode potential. The controllable peristaltic pump or flow regulating device is connected to a control interface to regulate the wastewater flow rate and hydraulic residence time. An electric field is applied between the electrodes, and hydroxyl radicals are generated in situ at the anode. Through convection-enhanced mass transfer, organic matter in the wastewater is transported to the anode surface to achieve mineralization, thereby achieving efficient and low-consumption deep treatment of the wastewater.

[0056] Fluorescent probe preparation: The fluorescent probe is TA, prepared in a pH 4.0-4.5 buffer solution, and placed in a bypass microfluidic channel (flow rate 0.2-1.0 mL / min). -1 The microfluidic channel is used to capture hydroxyl radicals in real time and generate HTA fluorescence signals. The microfluidic channel is preferably co-doped with an encapsulated inert fluorescent reference material (such as SiO2-coated quantum dots or carbon quantum dots) to achieve ratiometric self-calibration, and is covered with a hydrophobic barrier film (such as Nafion film) to reduce the interference of metal ions, free chlorine and natural organic matter on the fluorescence signal.

[0057] Optical module installation and calibration: The optical module includes a constant illuminance ultraviolet light source (approximately 315 nm) and a bandpass filter detector (425-430 nm, PMT or CCD / CMOS collector); a mapping relationship between fluorescence intensity and hydroxyl radical concentration is established using a standard HTA solution, and the mapping model is stored in the controller or host computer so that the algorithm program can be loaded in the data processing unit;

[0058] Closed-loop algorithm solution and control: The controller receives fluorescence signals in real time, extracts instantaneous ·OH concentration feature information through graph neural network, and adjusts power supply current density, electrode potential and wastewater flow rate through model prediction control algorithm to realize self-feedback dynamic regulation of electrolysis parameters and interface mass transfer-reaction process, avoiding insufficient ·OH due to excessively low current or side reactions and increased energy consumption caused by excessively high current;

[0059] Real-time monitoring and control device: The hardware components of the device include an industrial computer or embedded controller, a data acquisition card, an optical signal interface, a DC power supply interface, and a pump control interface; the controller exchanges data with each unit via wired (Ethernet, RS485) or wireless (Wi-Fi, Bluetooth) communication; the control program realizes signal acquisition, data processing, model predictive control calculation, and closed-loop output; the fluorescence signal is preprocessed (filtered, background subtraction, ratiometric) and then input into the control algorithm to adjust the power output and pump flow rate in real time, realizing dynamic adaptive matching of interface mass transfer and hydroxyl generation rate; the interface functions include: providing a real-time parameter monitoring interface, recording current density, electrode potential, flow rate, fluorescence intensity, calculated hydroxyl radical concentration and interface mass transfer-reaction state rate limiting step judgment, and realizing alarm output, operation log recording, and historical data analysis functions.

[0060] Long-term stability assurance measures: The platform can achieve anti-interference and self-cleaning through reference subtraction of background signal, timed acid washing and optical / temperature self-test; at the same time, two-point drift calibration is performed daily or weekly to ensure fluorescence quantization accuracy and closed-loop control reliability;

[0061] Platform Integration and Trial Operation: After completing modular integration, the intelligent platform will be launched for trial operation. Figure 2 This was used to verify the linkage between wastewater flow, electrolysis parameters, and fluorescence signals, ensuring that the platform has adaptive closed-loop control capabilities.

[0062] The specific implementation steps and operating results of Example 1 are as follows:

[0063] 1. Platform Construction and Preparation

[0064] The "Platform Construction and Preparation" of this embodiment is as follows: The self-feedback intelligent platform is modularly integrated from an electrochemical water treatment unit, a TA probe molecular fluorescence sensing unit, an optical acquisition and data processing unit, and an electro-hydraulic linkage online control unit, working collaboratively through a wired / wireless data interface. The electrochemical reactor adopts a through-type or tank-type structure, with the porous Ti4O7 anode and stainless steel cathode installed in parallel, preferably with a replaceable sealing gasket defining a 5-20 mm flow channel gap; a sampling port is set near the anode wall to lead the test liquid into the bypass microfluidic detection branch. A bypass microfluidic channel is set next to the electrolytic cell, with a flow rate of 0.2-1.0 mL·min. -1The process involves injecting TA (transferase in hydroxyl radical) online via a microfluidic pump to capture ·OH and generate HTA fluorescence signals. The optical module includes a constant-illuminance UV light source (center wavelength approximately 315 nm) and a bandpass filter detector (425-430 nm, PMT, CCD, or CMOS) for coaxial acquisition of HTA emission. A calibration curve of "fluorescence intensity - electrogenerated ·OH concentration" is established using a standard HTA solution, and the calibration model is loaded into the data processing unit of the controller or host computer. The controller reads the fluorescence data in real time, sequentially performing digital filtering, background subtraction, and ratiometric conversion. The algorithm calculates and applies a target current / voltage to the DC power supply and sets the flow rate of the peristaltic pump, achieving closed-loop linkage control of current density, anode potential, and flow rate to maintain a steady-state ·OH concentration that matches energy consumption and processing requirements. Execution and communication utilize an RS485 interface and Modbus protocol. The controller sends parameter commands to the DC power supply and peristaltic pump and records operating data for traceability and subsequent self-tuning.

[0065] 2. Schematic diagram of the electrocatalytic water treatment unit

[0066] The electrocatalytic water treatment unit in this embodiment is an electrocatalytic oxidation system. A porous Ti4O7 anode is fixed and installed parallel to the stainless steel cathode in a through-type or tank-type electrolytic cell. Preferably, a replaceable sealing gasket is used to limit the flow channel gap to form a stable, confined flow field. Raw water enters the collection chamber through the inlet and flows tangentially along the anode surface, forming laminar flow within the electrode gap and establishing a thin diffusion boundary layer near the anode wall, thereby enhancing mass transfer at the reaction interface.

[0067] On the Ti4O7 anode surface, water molecules generate hydroxyl radicals (·OH) in situ via the anodic polarization path, and the generation rate is directly related to the current density. The generated ·OH undergoes reactions with contaminants at the interface, diffusion and migration into the bulk liquid, and partial quenching, thus forming a dynamic equilibrium of "generation-mass transfer-reaction". Figure 3 Pollutant molecules diffuse from the bulk liquid to the anode surface under the drive of the flow field. The surface concentration and the bulk liquid concentration are determined by the boundary layer thickness and diffusion coefficient. By adjusting the current density, anode potential, and flow rate, the Muncol number corresponding to the real-time limiting current density of pollutant concentration at the electrode interface can be dynamically controlled, achieving the optimal match between hydroxyl radical generation and pollutant mass transfer.

[0068] To ensure the controllability of the interfacial reaction state, this platform has a sampling port on the side wall of the tank, which is connected to the bypass microfluidic channel (flow rate 0.2-1.0 mL·min). -1The concentration of hydroxyl radicals was detected and calibrated online using an HTA fluorescent probe. A DC power supply and a peristaltic pump were connected to the controller via RS485 / Modbus, enabling real-time adjustment of current density, anode potential, and flow rate to achieve closed-loop optimized control of interfacial mass transfer and reaction rate.

[0069] 3. Construction of fluorescence sensing unit for TA probe molecules

[0070] The TA probe molecular fluorescence sensing unit in this embodiment consists of a bypass microfluidic channel and an optical acquisition component: the bypass channel draws water from the near-wall sampling port of the anode in the electrochemical water treatment unit, with a preferred flow rate of 0.2-1.0 mL·min. -1 The system is sequentially connected in series: "sensing zone—optical acquisition zone—recirculation / emission," and can be recirculated with the main flow or discharged independently. The sensing zone employs an in-situ mixing type within the bypass microfluidic chip cavity, co-doping terephthalic acid (TA) with an inert fluorescent reference material (such as SiO2-coated quantum dots or carbon quantum dots) to form a ratiometric probe, and is coated with a hydrophobic Nafion barrier film to reduce interference from metal ions, free chlorine, and natural organic matter on the signal and suppress swelling. Hydroxyl radicals (·OH) in the sampling solution react in situ with TA to generate 2-hydroxyterephthalic acid (HTA), initiating emission enhancement; the reference channel provides an intensity reference to compensate for fluctuations in the optical path and flow rate. The optical acquisition area employs a constant-illuminance ultraviolet light source (center wavelength approximately 315 nm) for orthogonal excitation, and a bandpass filter detector (425-430 nm, equipped with a PMT or CCD / CMOS) coaxially collects the HTA signal and simultaneously acquires the reference intensity; the signal is then converted into a ratio I after A / D conversion. HTA / I ref Upload the package along with a timestamp. Figure 4 To achieve quantification, a calibration curve of "fluorescence ratio - ·OH concentration" is established using a standard HTA solution and written to the controller or host computer; during operation, the ratio is instantly converted into the equivalent ·OH concentration and returned to the electro-hydraulic linkage online control unit via the bus for closed-loop adjustment of current density, anode potential, and flow rate. Figure 2 ) .

[0071] 4. Platform Operation and Closed-Loop Control

[0072] The "Platform Operation and Closed-Loop Control" in this embodiment is as follows: During the startup phase, the controller acquires the raw fluorescence signal from the HTA / reference dual-channel bypass microfluidic channel, and sequentially performs digital filtering, background subtraction, and ratioing processing to form a ratio I. HTA / I ref The estimated value C of the real-time equivalent concentration of hydroxyl radicals was obtained by conversion based on a pre-set calibration model. t The Ct The steady-state concentration of hydroxyl radicals (C) estimated under electrolysis conditions and limiting current density constraints is compared with that obtained by other methods. lim The difference between the two values ​​is used as the kernel of the model predictive control algorithm, which combines the mass transfer-reaction kinetics model of the controlled object with a rolling optimization strategy to solve for the optimal control variable within the constraint set (current density, electrode potential, upper and lower limits of flow rate / residence time, and rate of rise / rate of change). Figure 5 , 6 Control commands are transmitted via RS485 / Modbus to the controllable DC power supply and peristaltic pump, enabling synchronized tuning of current density, anode potential, and flow rate. This ensures that the in-situ hydroxyl radical generation rate at the anode and the interfacial mass transfer rate are time-matched. To enhance robustness, the controller preferably sets the system response time to no more than 30 seconds and enables upper and lower limit hysteresis, inverse integral saturation, predictive / feedforward compensation, and a limiter to suppress noise amplification and actuator jitter. When abnormal thresholds such as sensor disconnection, signal saturation, overcurrent, or overvoltage occur, the system automatically enters a safety fallback mode (current or pressure limiting, flow rate reduction, or switching to conservative PI mode), while simultaneously logging events and archiving timestamps. Calibration curves and control parameters are version-managed, and key operating data is continuously recorded for traceability analysis and self-tuning updates, thereby maintaining the repeatability and long-term stability of closed-loop control under different influent water quality and load disturbance conditions.

[0073] 5. Low power consumption and system stability

[0074] The platform relies on a closed loop of "electrolysis parameters-fluorescence signal-model predictive control" to monitor the equivalent concentration of ·OH in real time during operation and adjust the current density, anode potential, and flow rate accordingly. This avoids ineffective energy consumption and amplification of side reactions caused by overcurrent, while also preventing interfacial mass transfer and reaction rate imbalances due to insufficient ·OH supply. Under validation conditions of 30 days of continuous operation, the intraday / interday fluctuations of fluorescence signal readings, COD removal rate, and current efficiency were all controlled within ±5%, and no significant observable accumulation of byproducts was detected. The controller can automatically adjust the current density and flow rate according to changes in influent water quality and load, reducing energy consumption per unit volume by approximately 28% compared to constant operating conditions. Figure 6 , 7The above operational results demonstrate that this platform possesses reliable adaptive control and energy consumption optimization capabilities under long-term continuous operation. Its system robustness stems from multi-source feedback ratiometric fluorescence measurement and reference channels, self-calibration and drift correction mechanisms, constraint-based electro / hydraulic bivariate coupling optimization, and fault-tolerant strategies including hysteresis, prediction / feedforward compensation, and limiting / backoff modes. In the event of sensor malfunctions, load disturbances, or fluctuations in influent water quality, the closed loop can recover to a stable trajectory within a set response time, ensuring stable, low-power, and repeatable operation under complex conditions, making it suitable for continuous engineering applications.

[0075] This specific embodiment is merely an explanation of the present invention and is not intended to limit the invention. After reading this specification, those skilled in the art can make modifications to this embodiment without contributing any inventive step, but such modifications are protected by patent law as long as they are within the scope of the claims of the present invention.

Claims

1. A method for constructing a self-feedback intelligent electrocatalytic wastewater treatment platform, characterized by: The construction method comprises the following steps: S1 Reactor and electrode construction: setting up an electrocatalytic anode that can generate ·OH, a cathode, a reference electrode, a programmable power supply, a programmable peristaltic pump or a flow regulating device, and an electrode surface sampling port; S2 Terephthalic acid probe molecule capture configuration: preparing an acidic buffer with a pH of 3.5-4.5 and a 0.1-1 mM terephthalic acid capture solution TA to capture the electrocatalytic active electrode surface to generate hydroxyl radicals specifically to produce hydroxylated terephthalic acid fluorescent product HTA; S3 Optical module installation and calibration: establishing a mapping model of fluorescence intensity and hydroxyl radical equivalent concentration in a constant-temperature dark box, and storing the calibration parameters in the controller; S4 Online sampling and in-situ fluorescence detection: The fluorescence signal is periodically collected through the bypass microfluidic channel or patch-type sensing unit, wherein the reaction microzone is provided with HTA and inert fluorescent reference material and covered with a hydrophobic barrier film, and the bypass channel flow rate is 0.2 to 1.0 mL·min -1 ; S5 Algorithm solving and closed-loop control: real-time calculation of the steady-state equivalent concentration of hydroxyl radicals, estimation of the interface mass transfer capacity based on the limiting current model to form a constraint, and adjustment of the electrolysis parameters through the model predictive control algorithm to realize self-feedback closed-loop control; S6 Anti-interference and self-cleaning: background subtraction and drift compensation are performed on the reference channel or internal reference, and acid washing / backflushing and optical and temperature self-checking are performed periodically; S7 Long-term drift calibration: two-point calibration is performed daily or weekly; Each step is implemented in parallel in the order to construct and operate the intelligent platform.

2. The smart platform constructed according to the construction method of claim 1, characterized in that: The intelligent platform is modularly integrated with an electrochemical water treatment unit, a terephthalic acid probe molecule fluorescence sensing unit, a signal acquisition and data processing unit, and an electro-hydraulic linkage online control unit; each unit communicates data through Ethernet or RS-485, and realizes pluggable integration through standardized electrical and fluid interfaces; the platform is used for online monitoring of the steady-state equivalent concentration of hydroxyl radicals and dynamic adjustment of electrolysis parameters under the constraint of the model predictive control algorithm, thereby realizing efficient, stable and energy-saving operation of the electrochemical oxidation process.

3. The intelligent platform of claim 2, wherein: The electrochemical water treatment unit is suitable for advanced wastewater treatment, and in-situ generation of hydroxyl radicals on the electrode interface through anodic electrocatalytic oxidation, cathodic electro-Fenton or their combination to realize deep mineralization of refractory organic pollutants; a bypass or in-situ microflow monitoring area is arranged adjacent to the electrogenerated hydroxyl radical electrode surface.

4. The intelligent platform of claim 3, characterized by: The anode is a boron-doped diamond, titanium suboxide, Ti / SnO2, Ti / PbO2, RuO2 or IrO2-based mixed metal oxide electrode; the cathode is a gas diffusion electrode, carbon felt, graphite felt, graphene-loaded electrode, or its surface is modified with iron-based single-atom catalyst, Fe-N-C material, Fe-MOF or iron sulfide-carbon composite material.

5. The intelligent platform of claim 2 or 3, characterized by: The terephthalic acid probe molecule fluorescence sensing unit is a bypass microfluidic channel or a patch-type gel sensing patch, the channel or patch contains a buffer system with a pH of 3.5-4.5 and a TA substrate, to specifically capture hydroxyl radicals and generate a fluorescent adduct product hydroxylated terephthalic acid; the terephthalic acid probe molecule fluorescence sensing unit is covered with a hydrophobic anti-interference barrier film and a reference branch is arranged for background subtraction; wherein the optical path of the bypass microfluidic channel is 1-2 mm, the channel flow rate is 0.2-1.0 mL·min -1 , the response time is ≤30 s; the patch-type gel sensing patch uses a PVA-alginate or polyacrylamide gel and encapsulates an inert fluorescent reference substance to achieve ratio-based self-calibration; and at the data processing end, the background subtraction before operation, drift compensation and ratio algorithm are implemented to improve the measurement accuracy of the steady-state hydroxyl equivalent concentration.

6. The intelligent platform of claim 2, wherein: The signal acquisition and data processing unit is in communication with the terephthalic acid probe molecule fluorescence sensing unit, used for pre-processing and quantitative fitting of the fluorescence signal, mapping the fluorescence signal to the steady-state equivalent concentration of hydroxyl radicals, and implementing matrix correction; the signal acquisition and data processing unit comprises a constant-illumination ultraviolet excitation light source and an emission bandpass filter element and a photodetector, the bandpass filter photodetector is PMT, CCD or CMOS, which acquires HTA fluorescence signal in the 425-430 nm waveband, and is arranged in a dark box or an integrating sphere to ensure uniform light collection.

7. The intelligent platform of claim 2, wherein: The signal acquisition data processing unit further comprises a temperature and illumination drift compensation module and a reference channel, and the intelligent platform can be configured in parallel with electrochemical detection of HTA products as a redundant signal to further improve the detection reliability of the fluorescence signal.

8. The intelligent platform of claim 2, wherein: The electric-hydraulic linkage online control unit comprises a programmable direct current power supply, a programmable peristaltic pump or a flow regulating device, a controller and an algorithm processing module, and is used for monitoring a reference electrode and a sampling interface of an electrode potential; data communication is performed through an Ethernet or RS-485 bus, and pluggable connection is realized through standardized electrical terminals and fluid joints; the controller receives the TA fluorescence sensing unit output signal in real time through image recognition, extracts real-time ·OH concentration feature information through a graph neural network, and calculates an output closed-loop control instruction based on a model predictive control algorithm.

9. The intelligent platform of claim 8, characterized by: The model predictive control algorithm combines real-time fluorescence sensing signals and actual electrolysis parameters, estimates the interface mass transfer capacity with the limit current density as a constraint, and solves the optimal control strategy in real time with the removal rate and unit energy consumption as the objective function, dynamically adjusts the current density, electrode potential and hydraulic retention time, so as to realize adaptive regulation of the interface hydroxyl generation rate and the pollutant mineralization rate under complex water quality conditions, and maintain stable operation with high efficiency and low energy consumption.

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