Kinetics Of Electrooxidation Research Articles

Optimizing Electro-Oxidation Kinetics via Constructing Built-In Electric Field on Pd-Ni(OH)2 Heterostructures for Selective Oxidation of Benzylamine to Benzonitrile.

Rationally regulating redox properties of electrocatalysts is highly essential to accomplish selective electro-oxidation of benzylamine (BA) to benzonitrile (BN) and concurrently promote hydrogen evolution reaction (HER) at cathode. Herein, a facile built-in electric field (BIEF) engineering strategy to optimize the electrocatalytic kinetics for the BA oxidation reaction (BOR) on Pd-Ni(OH)2 heterostructures, is presented. Both experimental and theoretical results confirm the construction of BIEF with the direction from α-Ni(OH)2 nanosheet to Pd nanoparticle at the heterointerface. It is unequivocally found that the creation of BIEF is favorable for not only the generation of electroactive Ni(OH)O species, but also the adsorption and dehydrogenation of BA molecules, achieving significantly promoted BOR kinetics. As expected, the Pd-Ni(OH)2 catalyst shows excellent electrocatalytic performance toward selectively oxidizing BA to BN, which is further coupled with cathodic H2 production. The faradaic efficiency (FE) for BN production can approximate to 85% in a two-electrode electrolyzer. In situ Raman spectroscopy and electrochemical measurements disclose that the activity origin for the BOR is dehydronated Ni(OH)O intermediate, clarifying a direct electro-oxidation mechanism over the Pd-Ni(OH)2 electrode. This work highlights an effective insight into design and synthesis of highly active electrocatalysts for organic upgrading.

Enhancing the Kinetics of Glucose Electro-Oxidation by Modulating the Binding Energy of Hydroxyl on Cobalt-Based Catalysts.

Replacing the sluggish anodic water oxidation reaction with the glucose oxidation reaction (GOR) offers an energy-saving strategy to obtain value-added products during the hydrogen production process. However, rational design of the GOR electrocatalyst with an explicit structure-property relationship remains a challenge. In this study, by using cobalt chalcogenides as model catalysts, we performed an in-depth study of the GOR catalytic mechanism of CoS and CoSe nanosheets. Experimental and theoretical results revealed that the reaction pathway on cobalt chalcogenides strongly depends on their binding energy to hydroxyl (OHBE). For CoS with a weak OHBE, the reaction proceeds through an "electrophilic oxygen" route. While for CoSe, due to the strong OHBE, a surface reconstruction occurs before the GOR and therefore follows the "electrochemical-chemical" route. Inspired by these findings, a customized strategy was proposed to regulate the OHBE of the catalysts, which involved introducing F atoms into CoS to enhance its OHBE, and weakening the OHBE of CoSe by doping with Zn atoms. The optimized F-doped CoS and Zn-doped CoSe catalysts both exhibited significantly improved performance for GOR. This study thus provides a verifiable paradigm for improving the GOR performance via a customized strategy and sheds light on the design of novel catalysts in the future.

Chitosan/platinum nanocubes/Mn(TPDCA)2-modified glassy carbon electrodes for the electrochemical quantification of amlodipine in unprocessed plasma samples

A novel electrochemical probe is developed to detect amlodipine (AMD) in unprocessed plasma samples. The fabrication process involves the synthesis of platinum nanocubes (Pt NCs) and Mn(TPDCA)2 complexes, which are then immobilized them onto the glassy carbon electrode (GCE) surface. The developed electrochemical probe demonstrates exceptional detection performance, with a wide dynamic range, outstanding selectivity, and commendable reproducibility. The linear range and lower limit of detection of the developed method are 53 nM-3.5 µM and 53 nM, respectively. Electrochemical experiments have been conducted to study the kinetics of electrooxidation on the modified electrode, revealing that the process is diffusion-controlled. Furthermore, method validation studies are performed to assess the accuracy, precision, and selectivity of the sensor, demonstrating excellent performance in all these aspects. Consequently, it can be concluded that the sensor is highly suitable for practical applications in drug analysis.

Water Electrooxidation Kinetics Clarified by Time‐Resolved X‐Ray Absorption and Electrochemical Impedance Spectroscopy for a Bulk‐Active Cobalt Material

AbstractWater oxidation, the oxygen evolution reaction (OER), is the anodic process in electrocatalytic production of hydrogen and further green fuels. Transition‐metal oxyhydroxides with bulk‐phase OER activity of the complete material or amorphized near‐surface regions are of prime application interest, but their basic electrochemical properties are insufficiently understood. Here the timescale of functional processes is clarified by time‐resolved X‐ray absorption spectroscopy and electrochemical impedance spectroscopy (EIS) for a thickness‐series of cobalt oxyhydroxides films (about 35–550 nm). At the outer material surface, an electric double‐layer is formed in microseconds followed by clearly cobalt‐centered redox‐state changes of the bulk material in the low millisecond domain and a slow chemical step of O2‐formation, within hundreds of milliseconds. Conceptually interesting, the electrode potential likely controls the OER rate indirectly by driving the catalyst material to an increasingly oxidized state which promotes the rate‐limiting chemical step. Rate constants are derived for redox chemistry and catalysis from EIS data of low‐thickness catalyst films; at higher thicknesses, catalyst‐internal charge transport limitations become increasingly relevant. Relations between electrochemically active surface area, double‐layer capacitance, and redox (pseudo‐)capacitance are discussed. These results can increase the power of EIS analyses and support knowledge‐guided optimization of a broader class of OER catalyst materials.

Voltammetric detection of chlorogenic acid by Poly(3,4-ethylene-dioxythiophene) electrodes

This work aims at developing selective detection of chlorogenic acid (CGA), a critical phenolic acid related to the antioxidant level and taste of coffee, by a pristine poly(3,4-ethylenedioxythiophene) (PEDOT) electrode. The electrochemical oxidation of CGA on two types of PEDOT films, electrodeposited in aqueous (water, aq-PEDOT) and non-aqueous solvents (acetonitrile, ACN-PEDOT), were systematically studied and compared. Aq-PEDOT film showed a linear response for CGA in a range from 1.5 µM to 2.5 mM and a sensitivity of 0.33 mA/cm2⋅mM; ACN-PEDOT film showed a non-linear response with residual CGA. For repeated sensing purposes, we chose aq-PEDOT for the CGA sensor demonstration. Although cross-sensitivity with gallic acid (GA) and caffeic acid (CA) at 0.35 V was observed due to the shared catechol structure, selectivity for CGA determination against vanillin (VAN), guaiacol (GUA), theobromine (THB), theophylline (THP), quinic acid (QA), and caffeine (CAF) was confirmed. The distinct sensing behavior of the PEDOT films was further investigated: aq-PEDOT had a relatively flat surface and obeyed diffusion-controlled kinetics for CGA electro-oxidation. In contrast, ACN-PEDOT had a rougher coral-like morphology and strong adsorption characteristics. The measurements in real coffee samples by aq-PEDOT were also demonstrated with the interference from CA compensated. In brief, this study proves the niches and provides in-depth electrochemical kinetics for voltammetric CGA sensing using the PEDOT films prepared in aqueous and non-aqueous environments.

Promoting role of Europium on Multi-Walled Carbon Nanotube (MWCNT) supported Platinum catalyst for Ethanol Electro-Oxidation in Direct Alcohol Fuel Cell (DAFC)

Implementing rare earth metals with platinum for Ethanol Oxidation Reactions (EOR) has received significant interest in the promising DEFC. Incorporation of Europium, a rare earth metal, influences the electron density of the Pt, and the resulting catalytic activity is reinforced. Herein, different molar ratios of binary PtEu electrocatalysts supported over MWCNT were synthesized using the borohydride reduction method. The purpose of the investigation was to determine how the atomic structure, composition, and activity of the electrocatalyst correlate to the EOR. Structure, bulk composition, morphology, and bonding of the electrocatalyst were investigated through X-ray diffraction (XRD), Scanning Electron Microscopy (SEM), Energy-Dispersive X-ray (EDX), Fourier Transform Infrared (FTIR) spectroscopy, and RAMAN spectroscopy. Cyclic Voltammetry (CV), Linear Sweep Voltammetry (LSV), chronoamperometry (CA), and Electrochemical Impedance Spectroscopy (EIS) techniques were employed to probe the electro-oxidation kinetics on the electrocatalyst's surface. During the EOR circumstances, the PtEu electrocatalysts showed a captivating composition-structure-activity relationship, consistent with the findings. Notably, all the physical and electrochemical analyses demonstrate that the bimetallic composition of the 84:16 electrocatalyst has shown higher EOR activity through a bifunctional mechanism. The results provide novel insights into the ethanol oxidation process over bimetallic alloy electrocatalysts, which is crucial for designing robust and efficient electrocatalysts for DEFC.

Harnessing the Potential of Hollow Graphitic Carbon Nanocages for Enhanced Methanol Oxidation Using PtRu Nanoparticles.

Direct Methanol Fuel Cell (DMFC) is a powerful system for generating electrical energy for various applications. However, there are several limitations that hinder the commercialization of DMFCs, such as the expense of platinum (Pt) at market price, sluggish methanol oxidation reaction (MOR) due to carbon monoxide (CO) formation, and slow electrooxidation kinetics. This work introduces carbon nanocages (CNCs) that were obtained through the pyrolysis of polypyrrole (Ppy) as the carbon source. The CNCs were characterized using BET, XRD, HRTEM, TEM, SEM, and FTIR techniques. The CNCs derived from the Ppy source, pyrolyzed at 750 °C, exhibited the best morphologies with a high specific surface area of 416 m2g-1, allowing for good metal dispersion. Subsequently, PtRu catalyst was doped onto the CNC-Ppy750 support using chemical reduction and microwave-assisted methods. In electrochemical tests, the PtRu/CNC-Ppy750 electrocatalyst demonstrated improved CO tolerance and higher performance in MOR compared to PtRu-supported commercial carbon black (CB), with values of 427 mA mg-1 and 248 mA mg-1, respectively. The superior MOR performance of PtRu/CNC-Ppy750 was attributed to its high surface area of CNC support, uniform dispersion of PtRu catalyst, and small PtRu nanoparticles on the CNC. In DMFC single-cell tests, the PtRu/CNC-Ppy750 exhibited higher performance, approximately 1.7 times higher than PtRu/CB. In conclusion, the PtRu/CNC-PPy750 represents a promising electrocatalyst candidate for MOR and anodic DMFC applications.

Kinetics of Electrooxidation of Dimethyl Sulfoxide on a Platinum Electrode with Sulphuric Acid and Alkaline Solutions

In this work, an electrochemical study of the mechanism of electrooxidation of dimethyl sulfoxide (DMSO) on a platinum electrode in acidic and alkaline solutions was carried out. On stationary polarization anodic curves taken within DMSO in an acidic and alkaline environment, the processing currents are processed manually than in dissolved light. When analyzing linear sections of anodic voltammograms, the values of the coefficients of the Tafel equation were achieved. This definition defines the current density measurement range and conditions for the electrooxidation of DMSO on a platinum (Pt) electrode. Electrolysis was carried out at controlled current densities in an electrolyzer without separation and with separation of the anode and cathode compartments using MK-40, MA-40 membranes and a fluoropolymer sulfcationite membrane MF-4SK. The high electrical conductivity and selectivity of the membranes ensures good performance of the electrolysis process and obtains a high-purity final product. Raman spectroscopy and gas chromatography-mass spectrometry have confirmed that the products of DMSO electrooxidation in an acidic environment are dimethyl sulfone (DMSO2) and methanesulfonic acid (MSA), and in an alkaline environment DMSO2 and sodium methanesulfonate. The method of quantum chemical calculations showed good adsorption of DMSO molecules on platinum within the framework of the cluster model. It has been established that the formation of MSA on the surface of a platinum electrode at high current densities occurs via the radical ion mechanism, by breaking the C–S bond. Based on the experimental results obtained, a scheme for the electrochemical oxidation of dimethyl sulfoxide on platinum is proposed.

Ethylenediamine-mediated synthesis of Pd-based catalysts with enhanced electrocatalytic performances towards formic acid oxidation

Pd-based anode catalysts with superior activity are urgent for formic acid oxidation to further boost the direct formic acid fuel cells (DFAFCs) technologies. Herein, a strategy of ethylenediamine (EDA) modified Pd/C catalyst was developed by two main steps of EDA adsorbed on Vulcan XC-72 carbon by impregnation and Pd nanoparticles loaded on the freeze-dried C-EDA supports by liquid reduction method. The effects of sweep rates and concentrations of EDA on the formic acid electrooxidation were systematically studied. Results showed that the above parameter was optimized as the concentration of EDA of 0.1 mol L−1. Pd nanoparticles with even distribution were fabricated and particle sizes were in the range of 3.5–4.2 nm. In addition, Pd particle size became smaller with the addition of EDA, suggesting that EDA could induce the generation of smaller Pd. Electrochemical measurements demonstrated that the electrocatalytic activity of Pd/C-0.22EDA (1021 mA mg−1) with optimized modification concentration was improved as a factor of 3.82 than that of Pd/C (267 mA mg−1). An enhanced stability (about 41 times higher than Pd/C) and faster charge-transfer kinetics of formic acid electrooxidation were observed for Pd/C-0.22EDA catalyst. CV and CA measurements showed that the most active catalyst was made of the smallest (3.5 nm) Pd nanoparticles for Pd/C-0.22EDA catalyst. The better electrocatalytic performances of Pd/C-0.22EDA might be ascribed to evenly dispersed Pd with relatively smaller particle size, electron regulation between Pd and amine group as well as stable Pd structure.

Kinetics of Formic Acid Electrooxidation on Anodically Modified Silver–Palladium Alloys

Kinetics of Formic Acid Electrooxidation on Anodically Modified Silver–Palladium Alloys

Promoted electro-oxidation kinetics in chromium-doped α‑Ni(OH)2 nanosheets for efficient selective conversion of methanol to formate

Owing to the elusive pathways of methanol oxidation reaction (MOR) and the lack of applicable catalysts, the selective electro-oxidation of methanol to formate remains a challenging topic. Herein, we present a chromium-doping strategy to promote the MOR performance of α-Ni(OH)2 nanosheets with a high selectivity towards formate generation. Taking chromium-doped α-Ni(OH)2 nanosheets as an example, we further highlight the role of doping atoms in MOR by combining theoretical calculations with experimental measurements. It reveals that chromium doping can not only enhance the conductivity of α-Ni(OH)2 nanosheets, but also endow the catalyst with optimized kinetics for electroactive NiOOH formation and methanol absorption, thus resulting in a remarkable MOR current density of 141 mA cm−2 at 0.50 V vs. Ag/AgCl with a faradaic efficiency of 92.1% for formate. Furthermore, in situ infrared spectroscopy demonstrates that methanol is selectively oxidized to formate without further oxidation to CO2 over chromium-doped α‑Ni(OH)2 nanosheets in alkaline media.

The progress of research on vacancies in HMF electrooxidation.

5-Hydroxymethylfurfural (HMF), serving as a versatile platform compound bridging biomass resource and the fine chemicals industry, holds significant importance in biomass conversion processes. The electrooxidation of HMF plays a crucial role in yielding the valuable product (2,5-furandicarboxylic acid), which finds important applications in antimicrobial agents, pharmaceutical intermediates, polyester synthesis, and so on. Defect engineering stands as one of the most effective strategies for precisely synthesizing electrocatalytic materials, which could tune the electronic structure and coordination environment, and further altering the adsorption energy of HMF intermediate species, consequently increasing the kinetics of HMF electrooxidation. Thereinto, the most routine and effective defect are the anionic vacancies and cationic vacancies. In this concise review, the catalytic reaction mechanism for selective HMF oxidation is first elucidated, with a focus on the synthesis strategies involving both anionic and cationic vacancies. Recent advancements in various catalytic oxidation systems for HMF are summarized and synthesized from this perspective. Finally, the future research prospects for selective HMF oxidation are discussed.

Nonredox trivalent nickel catalyzing nucleophilic electrooxidation of organics

A thorough comprehension of the mechanism behind organic electrooxidation is crucial for the development of efficient energy conversion technology. Here, we find that trivalent nickel is capable of oxidizing organics through a nucleophilic attack and electron transfer via a nonredox process. This nonredox trivalent nickel exhibits exceptional kinetic efficiency in oxidizing organics that possess the highest occupied molecular orbital energy levels ranging from −7.4 to −6 eV (vs. Vacuum level) and the dual local softness values of nucleophilic atoms in nucleophilic functional groups, such as hydroxyls (methanol, ethanol, benzyl alcohol), carbonyls (formamide, urea, formaldehyde, glucose, and N-acetyl glucosamine), and aminos (benzylamine), ranging from −0.65 to −0.15. The rapid electrooxidation kinetics can be attributed to the isoenergetic channels created by the nucleophilic attack and the nonredox electron transfer via the unoccupied eg orbitals of trivalent nickel (t2g6eg1). Our findings are valuable in identifying kinetically fast organic electrooxidation on nonredox catalysts for efficient energy conversions.

Shifting Emphasis from Electro- to Catalytically Active Sites: Effects of Pore Size of Flow-Through Anodes on Water Purification.

A flow-through anode has demonstrated high efficiency for micropollutant abatement in water purification. In addition to developing novel electrode materials, a rational design of its porous structure is crucial to achieve high electrooxidation kinetics while sustaining a low cost for flow-through operation. However, our knowledge of the relationship between the pore structure and its performance is still incomplete. Therefore, we systematically explore the effect of pore size (with a median from 4.7 to 49.4 μm) on the flow-through anode efficiency. Results showed that when the pore size was <26.7 μm, the electrooxidation kinetics was insignificantly improved, but the permeability declined dramatically. Traditional empirical evidence from hydrodynamic modeling and electrochemical tests indicated that a flow-through anode with a smaller pore size (e.g., 4.7 μm) had a high mass transfer capability and large electroactive area. However, this did not further accelerate the micropollutant removal. Combining an overpotential distribution model and an imprinting method has revealed that the reactivity of a flow-through anode is related to the catalytically active volume/sites. The rapid overpotential decay as a function of depth in the anode would offset the merits arising from a small pore size. Herein, we demonstrate an optimal pore size distribution (∼20 μm) of typical flow-through anodes to maximize the process performance at a low energy cost, providing insights into the design of advanced flow-through anodes in water purification applications.

Room-temperature and gram-scale constructed Cu@CuO with promoted kinetics for glucose electrooxidation in the Faraday process

Room-temperature and gram-scale constructed Cu@CuO with promoted kinetics for glucose electrooxidation in the Faraday process

Co-reduction assisted fabrication of PdCuTe nanowires for enhanced glycerol electrooxidation

High-performance electrocatalysts for glycerol oxidation are highly craved for the direct glycerol fuel cells. Herein, trinary PdCuTe nanowires with well-defined nanostructure was prepared through a co-reduction assisted approach with Te nanowires as the starting template. The addition of ascorbic acid is the key for introduction of Cu into the PdTeCu nanowires during synthesis. Electrochemical results revealed that the incorporation of Cu could enhance the performance for glycerol electrooxidation, which rendering the as-fabricated PdCuTe nanowires afford the highest current density of 61.1 mA cm−2. Owe to the improved electrooxidation kinetics and reduced charge transfer resistance, the resultant PdCuTe nanowires also demonstrated a better long-term stability. The synthetic strategy proposed herein is useful for the preparation of other materials, and the developed catalysts herein may also find wide applications in electrochemical-related fields.

Nanozymes based on octahedral platinum nanocrystals with {111} surface facets: glucose oxidase mimicking activity in electrochemical sensors

The ability of shape-controlled octahedral Pt nanoparticles to act as nanozyme mimicking glucose oxidase enzyme is reported. Extended {111} particle surface facets coupled with a size comparable to natural enzymes and easy-to-remove citrate coating give high affinity for glucose, comparable to the enzyme as proven by the steady-state kinetics of glucose electrooxidation. The easy and thorough removal of the citrate coating, demonstrated by X-ray photoelectron spectroscopy analysis, allows a highly stable deposition of the nanozymes on the electrode. The glucose electrochemical detection (at −0.2 V vs SCE) shows a linear response between 0.36 and 17 mM with a limit of detection of 110 μM. A good reproducibility has been achieved, with an average relative standard deviation (RSD) value of 9.1% (n = 3). Similarly, a low intra-sensor variability has been observed, with a RSD of 6.6% (n = 3). Moreover, the sensor shows a long-term stability with reproducible performances for at least 2 months (RSD: 7.8%). Tests in saliva samples show the applicability of Pt nanozymes to commercial systems for non-invasive monitoring of hyperglycemia in saliva, with recoveries ranging from 92 to 98%.Graphical

(Invited) Kinetic Modeling of Ethanol Electro-Oxidation on Co-Ni-Mo-P Electrocatalyst

A rotating disk electrode technique was used to study the kinetics of ethanol electro-oxidation on multi-alloy composition of CoNiMoP deposited on catalyzed carbon substrate (CCS). A simple kinetic model for ethanol oxidation on CoNiMoP/CCS was developed with the assumption of a simultaneous generation of two main products – CH3CHO (acetaldehyde) and CH3COOH (acetic acid) and the experimental result was used to evaluate the kinetic parameters of the model. In the developed model, if only one of the two products- CH3CHO or CH3COOH was generated, the result showed that at high ethanol concentration, the ethanol reaction mechanism followed the acetaldehyde route while at low ethanol concentration, the mechanism led to acetic acid and carbon dioxide route. However, a modified model in which a simultaneous production of both CH3CHO and CH3COOH occurred, showed that ethanol oxidized rapidly to CH3COOH. Additionally, the effect of the rotation speed (400 or 900 rpm) on the reaction was investigated and the result showed that the speed did not affect the mechanism because the experimental results were closer to the CH3COOH curves for both cases (400 and 900 rpm), but rotation speed affected the mole fraction of CH3COOH and CH3CHO.

(Digital Presentation) Ethanol Electro-Oxidation Kinetics Using Activated Carbon-Supported Pt-Ag Catalysts in Alkaline Media

Due to scarcity of fossil fuels and their severe environmental consequences, the development of high efficiency energy conversion devices such as fuel cells (FCs) have gained considerable attention. The specific energy conversion efficiency of FC is highly influenced by the activity of the electrocatalysts. The Pt is widely used as an electrocatalyst due to its high activity and stability, but its high cost and depletion of resources hinder its commercialization. One of the workable strategies for the practical application of Pt is to reduce its content by alloying with some non-precious metals and simultaneously maintain its electrochemical performance. In this context, we developed a low Pt-loaded Pt-Ag/C alloy electrocatalyst via a gradual reduction process. The electrochemical performance of the as-synthesized catalyst was investigated by cyclic voltammetry (CV), linear sweep voltammetry (LSV), chronoamperometry (CA), and electrochemical impedance spectroscopy (EIS) using the three-electrode electrochemical workstation at room temperature. The electrocatalytic investigations reveal that the resultant alloy has an activity of 32.7 mA cm-2, which is significantly higher than that of Pt/C (17.6 mA cm-2) in an alkaline electrolyte and makes it a very efficient electrocatalyst for the ethanol oxidation reaction (EOR). The partial electron transfer from Ag to Pt in Pt-Ag alloy, which weakens the CO binding and poisoning effect on the surface, may be partly responsible for the enhanced catalytic activity of Pt-Ag/C. The activated carbon support also favors charge transport by transferring charge from catalytic active sites to external circuits. The stability and durability studies reveal that Pt-Ag/C performs significantly better than Pt/C, making it a viable electrocatalyst for EOR. Keywords: Direct Ethanol Fuel Cell, Electrochemical Impedance Spectroscopy, Cyclic Voltammetry, Alloy.

Enhanced dehydrogenation kinetics for ascorbic acid electrooxidation with ultra-low cell voltage and large current density

Dehydroascorbic acid (DHA) production from ascorbic acid electrochemical oxidation (AAOR) can be used to upgrade biomass derivatives and hydrogen production with low energy consumption. Carbon materials are a promising class of nonmetal AAOR electrocatalysts; however, their performance does not meet the requirements for practical applications. In this study, an oxygen-containing group (OCG)-modified carbon electrocatalyst was prepared via oxygen plasma treatment. It could drive a current density of 100 mA cm−2 at only 0.65 VRHE and realize a Faradaic efficiency of over 90% for DHA production with long-term stability of 20 h. A proton exchange membrane-type electrolyzer integrating the anodic AAOR and the cathodic hydrogen evolution reaction (HER) was assessed. It only requires a cell voltage input of 0.98 V to deliver a current density of 1000 mA cm−2, which is superior to most reported organic upgrading reactions. Moreover, it only needs 1.54 kWh to produce normal cubic H2, which is one-third of that of traditional water electrolysis. Importantly, the contribution of each type of OCG was investigated by combining electrochemical measurements and theoretical calculations. It was revealed that the OCGs, especially the carboxyl groups (–COOH) of carbon materials, could enhance the dehydrogenation kinetics of the AAOR, thereby boosting the electrocatalytic activity. This study presents a low-energy and eco-friendly strategy for electrochemical biomass upgrading and hydrogen production, provides an in-depth understanding of the role of oxygen-containing functional groups in the AAOR, and guides the design of carbon-based electrocatalysts for AAOR.