mA Cm-2 Research Articles

Epitaxial Growth of a Three-Dimensional Hollow and Chestnut Shell Photothermal p-n Junction Photoanode.

The p-n junction, a widely studied semiconductor material structure, offers only limited improvements in photoelectrochemical (PEC) efficiency. Herein, a three-dimensional (3D) p-n junction h-Ta3N5@CoN featuring a stable chestnut shell hollow sphere structure and photothermal effect was synthesized by using an epitaxial growth strategy. The fine fibers within the sphere induce Rayleigh scattering, which scatters unabsorbed light, thereby enabling secondary absorption and enhancing light utilization. The quantum confinement effects generated by CoN fine fibers, which are sized in a few nanometers, inhibit the recombination of electron-hole pairs. Moreover, the lattice matching between Ta3N5 and CoN allows for smoother movement of carriers and nonradiative relaxation phonons along the lattice, thereby enhancing the transport of both carriers and heat. The obtained h-Ta3N5@CoN/FTO p-n junction photoanode, under near-infrared (NIR) auxiliary irradiation, demonstrates a photocurrent of 8.71 mA cm-2 at 1.23 VRHE. Moreover, the h-Ta3N5@CoN+NIR/FTO photoanode can sustain operation for 168 h, which, to my knowledge, surpasses the operational durations of all other Ta3N5-based photoanodes. This study synthesizes three-dimensional hollow chestnut shell photothermal p-n heterojunctions through an epitaxial growth strategy, endowing the material with a more efficient carrier separation and photothermal transfer efficiency.

Photocatalytic Seawater Splitting by Earth-Abundant Catalysts: Metal-Semiconductor Metamaterials Made of Plasmonic Magnesium Diboride and Transitional Metal Dichalcogenides.

Metal-semiconductor metamaterials hold great promise for photocatalytic water splitting due to their excellent light harvesting in a broad spectral range as well as efficient charge carrier generation and transfer. In the majority of such metamaterials, semiconductors are used to initiate the water splitting reaction, while their metal counterparts are employed to improve light harvesting through plasmonic effects. Here, we describe for the first time an exceptional reversed case of metal-semiconductor photocatalysts in which metals are used to initiate the water splitting reaction and semiconductors are employed to improve light harvesting through the blackbody effect and serve as co-catalysts. The studied photoanodes are made of non-noble plasmonic MgB2 combined with transition metal dichalcogenides (TMDCs). The plasmonic resonances of the MgB2 component contribute to field confinement, plasmon-exciton coupling, and hot-electron transfer providing an enhancement of photoactivity in the entire solar spectrum capable of water splitting. The TMDC component provides impedance matching and enhances light absorption by the metal catalyst. We demonstrate seawater splitting with MgB2-TMDCs photoanodes attaining current densities of ~3 mA cm-2 at solar radiation. The overall efficiency of hydrogen production in seawater splitting by sunlight with the help of the studied photoanodes is 3 % at a bias voltage of Vbias=0.3 V.

Ni- and Co-Based MOF-Derived NixCo3-xO4 Materials: As an Efficient Anode for Direct Methanol Fuel Cell Application.

Finding inexpensive and efficient anode materials is crucial for the oxidation of methanol in the direct methanol fuel cell (DMFC), which is the key electrode reaction. Herein, we report metal-organic framework (MOF)-derived Co3O4, NiO, and NixCo3-xO4 (where x = 1.5, 1, and 0.6) materials deposited on nickel foam as efficient anode material for methanol oxidation. Among them, NiCo2O4 exhibited the highest methanol oxidation activity, owing to its lowest charge-transfer resistance (0.097 Ω) and high electrochemically active surface area (1950 cm2), resulting in the lowest onset potential of 0.35 V vs Hg/HgO. The optimized Ni-to-Co ratio and synergistic effect between Ni and Co metals enable NiCo2O4 to achieve the highest mass activity of 151 mA mg-1 and geometric current density of 288 mA cm-2, demonstrating excellent durability over 14 h at 0.6 V. In addition, to optimize methanol concentration, all the electrocatalysts were tested in a range of methanol concentrations, showing 0.5 M methanol as the optimal concentration. This study focuses on optimizing the metal ratio and methanol concentration to achieve the highest catalytic activity. Additionally, this lays the foundation for developing diverse MOF-derived electrocatalysts and advancing DMFCs.

A Novel Anion Receptor Additive for -40ºCSodium MetalBatteriesby Anion/Cation Solvation Engineering.

Sodium metal batteries, known for their high theoretical specific capacity, abundant reserves,and promisinglow-temperature performance, have garnered significant attention. However, the large ionic radius of Na+and sluggish transport kinetics across the interfacial structure hinder their practical application.Previous reviews have rarely regulated electrolyte performance from the perspective of anions; as important components of the electrolyte, the regulation mechanism is not well understood. Herein, a novel anion receptor additive, 4-aminophenylboronic acid pinalol ester (ABAPE), is proposed to weaken the coupling between anions and cations and accelerateNa+transport kinetics.The results of theoretical calculations and X-ray photoelectron spectroscopy with deep Ar-ion etching demonstrate thatthe introduction of this additive alters the solvation structure of Na+, reducesthe desolvation barrier and formsa stable and dense electrode-electrolyte interface. Moreover, ABAPE forms hydrogen bonds (-NH···O/F) with H2O/HF, effectively preventing the hydrolysis of NaPF6and stabilizing acidic species. Consequently, the Na||Na symmetric cell exhibits excellent long-cycle performance of 500 h at 1 mA cm-2 and 0.5 mAh cm-2. The Na||Na3V2(PO4)3(NVP) full cell with the addition of ABAPE maintains a capacity retention of 84.29% at 1 C after1200 cycles and presents no capacity decayover 150 cycles at -40°C.

Metal-organic framework-derived nanoflower and nanoflake metal oxides as electrocatalysts for methanol oxidation.

The energy crisis is the most urgent issue facing contemporary society and needs to be given top priority. As energy consumption rises, environmental pollution is becoming a serious issue. Direct methanol fuel cells (DMFCs) have emerged as the most promising energy source for a variety of applications such as electric vehicles and portable devices. Unfortunately, the kinetics of methanol oxidation is slow and needs an electrocatalyst to improve the reaction kinetics and the overall fuel cell efficiency. Herein, a straightforward hydrothermal procedure was utilized to prepare copper, nickel, and cobalt-based MOF composites by altering the elemental molar ratios. Cu-MOF (MOFP1), Cu/Ni-MOF (MOFP2), and Cu/Ni/Co-MOF (MOFP3) were prepared after carbonization and characterized using several key techniques such as FTIR, XRD, SEM, and EDX. The SEM analysis reveals that the morphology of MOFP1 is spherical aggregated particles, while that of MOFP2 or MOFP3 is in the form of nanoflakes and nanoflowers. Moreover, upon application of these composites as electrocatalysts for methanol electro-oxidation in an alkaline medium of 1 M NaOH using cyclic voltammetry (CV) and chronoamperometry (CA) tests, the electrochemical performance of MOFP2 in 1 M methanol exhibits the best performance for methanol oxidation with a current density reaching 38.77 mA cm-2 at a scan rate of 60 mV s-1. This can be attributed to the unique porous open flower structure and the synergistic effect between copper, nickel, and 2-aminoterephthalic acid which develop its catalytic activity.

Valence Band-Tunable NiFe Electrocatalyst Triggered by the Dynamic Mo Exudation and Re-Deposition for Superior High Current Density Oxygen Evolution Reaction.

Developing energy- and time-efficient strategies to derive high-performance non-precious electrocatalysts for anodic oxygen evolution reaction (OER), especially stably working at industrial-demanding current density, is still a big challenge. In this work, a concise molten salt erosion scenario was devised to rapidly modulate the smooth surface of the commercial NiMo foam substrate into the rough, electronically coupled, and hierarchically porous Ni/Fe/Mo(oxy)hydroxide catalyst layer assembled by the nanosphere array. This self-supported catalyst is super-hydrophilic for the alkaline electrolyte and distinguished by a balanced Mo leaching/surface-readsorption process to tune the metal d band center and electronic perturbation. The altered electronic environment with the favored OER intermediate adsorption behavior attains the outstanding OER activity in terms of a very small overpotential of 230.21 mV at 10 mA cm-2 and an ultra-long stability for 1179.45 h to sustain the initial commercial-level current density of ca. 1000 mA cm-2. This superb performance transcends most of the edge-cutting transition metal peers reported recently and can satisfy the standards of industrial applications. This industrial-compatible synthesis technology holds profound implications for hydrogen production via water splitting and other electrochemical applications.

Synchronous interlayer and surface engineering of NiFe layered double hydroxides by functional ligands for boosting oxygen evolution reaction

NiFe layered double hydroxides (LDHs) are among the most advanced electrocatalysts for oxygen evolution reaction (OER), but their catalytic activity and long-term working stability still need to be highly boosted for practical applications. Herein, an innovative strategy that combines anion intercalation/deintercalation and surface coordination is developed, which simultaneously realizes the modification of the interlay and surface properties of the NiFe LDHs by ethylenediaminetetraacetate (EDTA) and trisodium citrate (TSC). The intercalation/deintercalation of the anions engineers the interlay structure, while the surface metal-ligand coordination tunes the surface properties. Both the EDTA- and TSC-engineered NiFe LDHs exhibit highly enhanced catalytic performance, showing an overpotential of 204 and 233 mV, respectively at 10 mA cm-2 in 1.0 M KOH. The remarkable catalytic performance of the EDTA-engineered NiFe LDHs is due to the combined effect of the intercalation/deintercalation and the surface metal-EDTA coordination, while the surface TSC coordination only shows limited promoting effect on catalytic activity. In addition, the EDTA-engineered NiFe LDHs demonstrate good working stability at 100 mA cm-2.

Constructing Hydrangea-Like Iron-Cobalt Phosphides via Boron-Assisted Strategy as an Efficient Catalyst for Water Splitting at High Current Density.

Finding suitable bifunctional catalysts for industrial hydrogen production is the key to fully building a hydrogen energy society. In this study, we present a novel approach to modifying the surface morphology of electrodeposited cobalt phosphide (CoP). Specifically, we have developed a method to create a hydrangea-like structure of bimetallic cobalt-iron phosphide (B-CoFeP@CoP) through ion-exchange and NaBH4-assisted strategies. This catalyst exhibited excellent bifunctional catalytic capability at high current densities, achieving a current density of 500 mA cm-2 at a small overpotential (387 mV for OER and 252 mV for HER). When assembled into an OWS electrolyzer, this catalyst showed a fairly low cell voltage (≈1.88 V) at 500 mA cm-2 current density., Furthermore, B-CoFeP@CoP shows ceaseless durability over 120 h in both freshwater and seawater with almost no change in the cell voltage. A combined experimental and theoretical study identified that the unique hydrangea-like structure provided a larger electrochemically active surface area and more effective active sites. Further analysis indicates that during the OER process, phosphides ensure that bimetallic active sites adsorb more OOH * intermediates and further DFT calculations showed that B-Fe2P and B-Co2P acted as active centers for dissociation of H2O and desorption of H2, respectively, to synergistically catalyze the HER process.

Preserving Molecular Tuning for Enhanced Electrocatalytic CO2-to-Ethanol Conversion.

Modifying catalyst surface with small molecular-additives presents a promising avenue for enhancing electrocatalytic performance. However, challenges arise in preserving the molecular-additives and maximizing their tuning effect, particularly at high current densities. Herein, we develop an effective strategy to preserve the molecular-additives on electrode surface by applying a thin protective layer. Taking 4-dimethylaminopyridine (DMAP) as an example of a molecular-additive, the hydrophobic protection layer on top of the DMAP-functionalized Cu-catalyst effectively prevents its leaching during CO2 electroreduction (CO2R). Consequently, the confined DMAP molecules substantially promote the CO2-to-multicarbon conversion at low overpotentials. For instance, at a potential as low as -0.47 V vs. reversible hydrogen electrode, the DMAP-functionalized Cu exhibits over 80 % selectivity towards multi-carbon products, while the pristine Cu shows only ~35 % selectivity for multi-carbon products. Notably, ethanol appears as the primary product on DMAP-functionalized Cu, with selectivity approaching 50 % at a high current density of 400 mA cm-2. Detailed kinetic analysis, in situ spectroscopies, and theoretical calculations indicate that DMAP-induced electron accumulations on surface Cu-sites decrease the reaction energy for C-C coupling. Additionally, the interactions between DMAP and oxygenated intermediates facilitate the ethanol formation pathway in CO2R. Overall, this study showcases an effective strategy to guide future endeavors involving molecular tuning effects.

C3N4/Se-CNTs as Advanced Metal-Free Catalysts for the Photoassisted Electrocatalytic Oxygen Evolution Reaction.

Photoassisted electrocatalysis is a frontier direction of electrocatalysis for promoting energy conversion. In this work, a metal-free C3N4/Se-CNTs is reported as a novel catalyst for photoassisted electrocatalytic oxygen evolution reaction (OER). C3N4 has an appropriate bandgap, high specific surface area, and long-term stability. CNTs can modulate the electronic environment of C3N4 by strong π-π interaction and greatly enhance the separation efficiency of photogenerated carriers. The distributed Se nanoparticles in CNTs can further increase the charge transfer ability. As a metal-free catalyst, the C3N4/Se-CNTs exhibits an overpotential of 231 mV at a current density of 10 mA cm-2 and a small Tafel slope of 52 mV dec-1 under illumination, which ranks among the best catalysts for photoassisted OER performance, surpassing most noble and transition metal-based catalysts. The result demonstrates the great potential of C3N4-based catalysts in the photoassisted OER process and provides a new perspective to explore the excellent metal-free OER catalysts.

Oxygen Plasma Triggered Co-O-Fe Motif in Prussian Blue Analogue for Efficient and Robust Alkaline Water Oxidation.

In the context of oxygen evolution reaction (OER), the construction of high-valent transition metal sites to trigger the lattice oxygen oxidation mechanism is considered crucial for overcoming the performance limitations of traditional adsorbate evolution mechanism. However, the dynamic evolution of lattice oxygen during the reaction poses significant challenges for the stability of high-valent metal sites, particularly in high-current-density water-splitting systems. Here, we have successfully constructed Co-O-Fe catalytic active motifs in cobalt-iron Prussian blue analogs (CoFe-PBA) through oxygen plasma bombardment, effectively activating lattice oxygen reactivity while sustaining robust stability. Our spectroscopic and theoretical studies reveal that the Co-O-Fe bridged motifs enable a unique double-exchange interaction between Co and Fe atoms, promoting the formation of high-valent Co species as OER active centers while maintaining Fe in a low-valent state, preventing its dissolution. The resultant catalyst (CoFe-PBA-30) requires an overpotential of only 276 mV to achieve 1000 mA cm-2. Furthermore, the assembled alkaline exchange membrane electrolyzer using CoFe-PBA-30 as anode material achieves a high current density of 1 A cm-2 at 1.76 V and continuously operates for 250 hours with negligible degradation. This work provides significant insights for activating lattice oxygen redox without compromising structure stability in practical water electrolyzers.

Interface Synergistic Effect of NiFe-LDH/3D GA Composites on Efficient Electrocatalytic Water Oxidation.

Currently, NiFe-LDH exhibits an excellent oxygen evolution reaction (OER) due to the interaction of the two metal elements on the layered double hydroxide (LDH) platform. However, such interaction is still insufficient to compensate for its poor electrical conductivity, limited number of active sites and sluggish dynamics. Herein, a feasible two-step hydrothermal strategy that involves coupling low-conductivity NiFe-LDH with 3D porous graphene aerogel (GA) is proposed. The optimized NiFe-LDH/GA (1:1) produced possesses a 257 mV (10 mA cm-2) overpotential and could operate stably for 56 h in an OER. Our investigation demonstrates that the NiFe-LDH/GA has a three-dimensional mesoporous structure, and that there is synergistic interaction between LDH and GA and interfacial reconstruction of NiOOH. Such an interface synergistic coupling effect promotes fast mass transfer and facilitates OER kinetics, and this work offers new insights into designing efficient and stable GA-based electrocatalysts.

Structural Regulation of a Multi-Component Co2P2O7-MoN/NC Electrocatalyst for Efficient Oxygen Evolution Reaction.

Realizing efficient and durable non-precious metal-based electrocatalysts for oxygen evolution reaction (OER) still remains a great challenge. Here, a multi-component composite of Co2P2O7-MoN/NC containing pyrophosphate, nitride, and nitrogen-doped carbon is successfully prepared via a facile two-step synthesis method. Combining the structural regulation between the active metal- and non-metal-based species, Co2P2O7-MoN/NC demonstrates superior activity and durability for OER, requiring an overpotential of 278 mV at a current density of 10 mA cm-2, a Tafel slope of 83.3 mV dec-1, and long-term stability over 100 h in an alkaline solution. Post-characterizations reveal that synergistic effect among stable Co2P2O7, partially dissolved MoN, N-doped carbon, and new-formed CoOOH nanosheets enable structural reconstruction, fast charge transfer, and formation of oxygen-containing intermediates, promoting the OER performance significantly. This work provides a promising pathway to tune multi-components to fabricate efficient transition-metal-based electrocatalysts in energy conversion applications.

Oxyanions Enhancing Crystallinity of Reconstructed Phase for Oxygen Evolution Reaction.

The catalysts were always undergoing continuous amorphization and dissolution of active structure in operating condition, hindering the compatibility between stability and activity for oxygen evolution reaction (OER). Herein, we propose the selective adsorption of leached NO3- to strengthen the crystallinity and activity of surface reconstructed layer with amorphous and crystalline (a-c) heterojunction. Taking a-c Ni doped Fe2O(OH)3NO3·H2O (Ni-FeNH) as a model precatalyst, we uncover that the leached NO3- are readily adsorbs on the crystalline phase in the formed a-c Fe(Ni)OOH during OER, lowering the disorder degree and further activating Ni and Fe ion of the crystalline Fe(Ni)OOH on a-c heterojunctions. Accordingly, Ni-FeNH deliver a low overpotential of 303 mV and high durability of 500 hours at 500 mA cm-2 for OER. Particularly, constructing industrial water electrolysis equipment exhibits high stability of 100 hours under a high operating current of 8000 mA.

Next-Generation BiOCl/MXene Nanocomposites: Optimized for Dye Removal and Supercapacitor Applications.

The study focuses on the development of an efficient and sustainable solution for synthetic dye degradation through the hydrothermal synthesis of BiOCl and BiOCl/MXene heterostructures. Structural and compositional properties were analyzed by using X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), field emission scanning electron microscopy (FESEM), and X-ray photoelectron spectroscopy (XPS) techniques. A significant reduction in the band gap of BiOCl/MXene to 2.97 eV from 3.62 eV for BiOCl was observed via UV spectroscopy, leading to enhanced photocatalysis with 89% degradation efficiency in just 12 min. The mechanism involved and reactive species were confirmed by LC-HRMS and radical trapping tests, while ICP-MS verified metal content in water before and after degradation. Additionally, the nanocomposite demonstrated a specific capacitance of 431.24 F g-1 at a current density of 1 mA cm-2, with an excellent capacitance retention of 94.35% after 2000 cycles. This study highlights BiOCl/MXene as a promising material for both photodegradation and supercapacitor applications.

Constructing Cyclic Hydrogen Bonding to Suppress Side Reactions and Dendrite Formation on Zinc Anodes.

The high electrochemical reactivity of H2O molecules and zinc metal results in severe side reactions and dendrite formation on zinc anodes. Here we demonstrate that these issues can be addressed by using N-hydroxymethylacetamide (NHA) as additives in 2 M ZnSO4 electrolytes. The addition of NHA molecules, acting as both a hydrogen bond donor and acceptor, enables the formation of cyclic hydrogen bonding with H2O molecules. This interaction disrupts the existing hydrogen bonding networks between H2O molecules, hindering proton transport, and containing H2O molecules within the cyclic hydrogen bonding structure to prevent deprotonation. Additionally, NHA molecules show a preference for adsorption on the (101) crystal surface of zinc metal. This preferential adsorption reduces the surface energy of the (101) plane, facilitating the homogeneous Zn deposition along the (101) direction. Thus, the NHA enables Zn||Zn symmetric cell with a cycle lifespan of 1100 hours at 5 mA cm-2 and Zn||Cu asymmetric cell with a high Coulombic efficiency over 99.5 %. Moreover, the NHA-modified Zn||AC zinc ion hybrid capacitor is capable of sustaining 15000 cycles at 2 A g-1. This electrolyte additive engineering presents a promising strategy to enhance the performance and broaden the application potential of zinc metal-based energy storage devices.

Bismuth Nanoparticles and Single Iron Atoms on Carbon Derived from a Covalent Organic Framework Synergistically Catalyze the Oxygen Reduction Reaction.

The utilization of catalysts comprising metal nanoparticle has been beneficial for enhancing the performance of oxygen reduction reaction (ORR). However, the inadequate intrinsic activity of these catalysts still presents a significant challenge, limiting their overall effectiveness. This issue can be addressed by introducing single atoms, which can create a synergistic effect with the nanoparticles to catalyse and thereby improve performance. Nevertheless, the synergistic catalysis of nanoparticles and single atoms is still under investigation. In this study, we fabricated a core-shell structured carbon framework incorporating Fe single atoms and Bi nanoparticles through the pyrolysis of COF and MOF core-shell structures. Introducing Fe single atoms into ZIF-8, with Fe-ZIF-8 as the core and Bi-containing COF as the shell, resulted in higher ORR activity. The catalyst exhibited a half-wave potential of 0.867 V and a high current density of 6.68 mA cm-2 in 0.1 M KOH, which were comparable to those of Pt/C equivalent. This study provides new research concepts for exploring the application of single atoms and nanoparticles in catalytic oxygen reduction reactions through synergistic effects.

Electrokinetics of Nitrite to Ammonia Conversion in the Neutral Medium Over A Platinum Surface.

Polycrystalline Pt electrode was employed to selectively convert nitrite ions ( ) into useful nitrogenous compound through electrochemical reduction reaction in neutral medium. According to adsorptive stripping analysis, the reduction process produced nitric oxide (NO) on the surface of Pt electrode. The spectroscopic test and gas chromatographic studies discovered the presence of ammonia (NH3) in the electrolyzed solution, suggesting the transformation of adsorbed NO into NH3 during the reverse scan. Scan rate dependent investigation was performed to elucidate kinetic information relating to this reaction on Pt surface. From Ep vs scan rate (υ) and jp vs υ (logarithmic plot), it was found that the conversion of ion into NO is an irreversible reaction which relies on the diffusion of ions to electrode surface. The Tafel analysis unveiled that the first electron transfer sets the overall reaction rate, having formal reduction potential, E0'=-0.46 V and standard heterogeneous rate constant, k0= cm s-1. Reductive transfer coefficient (α) is another kinetics parameter, which was found to be approximate 0.77 from the difference between Ep and Ep/2 of the voltammograms obtained over scan rate range 0.005 V s-1 to 0.250 V s-1, indicating a stepwise process. According to temperature-dependent voltammograms, the nitrite reduction reaction on Pt had a calculated activation energy of about 19.8 kJ mol-1 and a pre-exponential factor of about 8.39×103 mA cm-2.

Self-Etching Synthesis of Superhydrophilic Iron-Rich Defect Heterostructure-Integrated Catalyst with Fast Oxygen Evolution Kinetics for Large-Current Water Splitting.

Developing catalysts with rich metal defects, strong hydrophilicit, and extensive grain boundaries is crucial for enhancing the kinetics of electrocatalytic water oxidation and facilitating large-current water splitting. In this study, we utilized pH-controlled etching and gas-phase phosphating to synthesize a flower-like Ni2P-FeP4-Cu3P modified nickel foam heterostructure catalyst. This catalyst features pronounced hydrophilicity and a high concentration of Fe defects. It exhibits low overpotentials of 156 mV and 210 mV at current densities of 10 and 100 mA cm-2 respectively, and maintains stability for up to 200 h at 100 mA cm-2 with only 7.3% degradation, showcasing outstanding electrocatalytic water oxidation performance. Furthermore, when integrated into a Ni2P-FeP4-Cu3P/NF||Pt-C/NF electrolyzer, it achieves excellent overall water splitting performance, reaching current densities of 10 and 400 mA cm-2 at just 1.47 V and 1.73 V, respectively, and operates stably for 60 h at 500 mA cm-2 with minimal degradation. Analysis indicates that high-valence oxyhydroxides/phosphides of Ni, Fe, and Cu act as the primary active species. The presence of abundant Fe defects enhances electron transfer, strong hydrophilicity improves electrolyte contact, and numerous grain boundaries synergistically modulate the activation energy between active sites and oxygen-containing intermediates, significantly improving the kinetics of water oxidation.

Direct Electrolysis of Municipal Reclaimed Water for Efficient Hydrogen Production Using a Bifunctional Non-Noble-Metal Catalyst.

Water electrolysis for green H2 production traditionally requires a stable supply of renewable electricity and pure water. However, spatial separation of renewables and water resources as well as water scarcity per capita in China necessitate unconventional water resources for electrolysis. Reclaimed water produced from municipal wastewater treatment plants is widely distributed with quality improved significantly in recent years, which may be a promising alternative to feedstock. However, there are few reports on the direct use of this wastewater for H2 production. Here, we present a direct electrolysis of reclaimed water for decentralized H2 production by developing a highly efficient and stable bifunctional 3D-dandelion-like (DL) vanadium(V)-doped CoP catalyst grown in situ on Ni foam (NF) in an alkaline electrolyzer. The V-CoP-DL/NF electrode decreases 6.5 and 25% overpotentials of the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively, compared to noble-metal Pt (HER) and IrO2 (OER) catalysts, and exhibits exceptional durability, as a voltage required for overall reclaimed water splitting only increases by 80 mV (1.81-1.89 V) after 90 days of operation at a current density of 10 mA cm-2. The maximum stable current can reach 1000 mA cm-2. The impacts of potential pollutants in reclaimed water on the performance of electrolysis and the behavior of major wastewater ions in alkaline electrolyte were investigated. The observed exceptional performance is attributed to the catalyst's unique nanostructure, which enhances charge transfer and reactant/electrolyte diffusion. The in situ growth strategy further enhances the conductivity and stability of the catalyst. This work underscores the feasibility of utilizing reclaimed water instead of pure water as the feedstock for sustainable hydrogen production.