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Co and Fe Codoped WO <sub/>2.72</sub> as Alkaline‐Solution‐Available Oxygen Evolution Reaction Catalyst to Construct Photovoltaic Water Splitting System with Solar‐To‐Hydrogen Efficiency of 16.9%
摘要： Oxygen evolution electrode is a crucial component of efficient photovoltaic-water electrolysis systems. Previous work focuses mainly on the effect of electronic structure modulation on the oxygen evolution reaction (OER) performance of 3d-transition-metal-based electrocatalyst. However, high-atomic-number W-based compound with complex electronic structure for versatile modulation is seldom explored because of its instability in OER-favorable alkaline solution. Here, codoping induced electronic structure modulation generates a beneficial effect of transforming the alkaline-labile WO2.72 (WO) in to efficient alkaline-solution-stable Co and Fe codoped WO2.72 (Co&Fe-WO) with porous urchin-like structure. The codoping lowers the chemical valence of W to ensure the durability of W-based catalyst, improves the electron-withdrawing capability of W and O to stabilize the Co and Fe in OER-favorable high valence state, and enriches the surface hydroxyls, which act as reactive sites. The Co&Fe-WO shows ultralow overpotential (226 mV, J = 10 mA cm?2), low Tafel slope (33.7 mV dec?1), and good conductivity. This catalyst is finally applied to a photovoltaic-water splitting system to stably produce hydrogen for 50 h at a high solar-to-hydrogen efficiency of 16.9%. This work highlights the impressive effect of electronic structure modulation on W-based catalyst, and may inspire the modification of potential but unstable catalyst for solar energy conversion.
关键词： electrocatalysis,photovoltaic water splitting,oxygen evolution reaction,codoping,WO2.72
更新于2025-11-14 17:04:02
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Gold doping induced strong enhancement of carbon quantum dots fluorescence and oxygen evolution reaction catalytic activity of amorphous cobalt hydroxide
摘要： Gold doping induced strong enhancement of carbon quantum dots fluorescence and oxygen evolution reaction catalytic activity of amorphous cobalt hydroxide. Water splitting using electrocatalysts is expected to provide an alternative green energy source to meet increasing energy demands as well as addressing environmental concerns related to fossil fuels. Herein, we report one-step synthesis of sulfur, nitrogen and Au-doped carbon quantum dots (Au-SCQDs) and strong enhancement of fluorescence intensity and oxygen evolution reaction (OER) catalytic activity of amorphous Co(OH)2 nanoparticles compared to pure Co(OH)2 as well as commercial RuO2 and Pt/C catalysts. Au doping into sulfur and nitrogen co-doped CQDs showed over seventy times enhanced fluorescence. OER studies of amorphous-Co(OH)2 incorporated Au-SCQDs produced current density of 178 mA cm?2 at the applied potential of 2.07 V whereas un-doped Co(OH)2 showed current density of 59 mA cm?2. To produce geometric current density of 10 mA cm?2, amorphous Co(OH)2-Au-SCQDs (CSA) required 388–456 mV overpotential depending on the Au ion concentration used for preparing the Au-SCQDs, which is equal to or lower than overpotential required by commercial electrocatalysts. The strongly enhanced OER activity of Co(OH)2-Au-SCQDs (CSA) was attributed to the presence of electronegative metallic conducting Au atoms along with the high catalytic surface area of amorphous Co(OH)2. The present studies demonstrate a new method of exploiting amorphous Co(OH)2NPs electrocatalysts that could provide more catalytically active sites by integrating an electronegative conducting Au atom doped SCQDs matrix.
关键词： amorphous cobalt hydroxide,fluorescence,water splitting,Gold doping,carbon quantum dots,oxygen evolution reaction,electrocatalysts
更新于2025-10-22 19:40:53
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Multi-active sites derived from a single/double perovskite hybrid for highly efficient water oxidation
摘要： The oxygen evolution reaction (OER) plays a crucial role in the application of water splitting, which is a highly competitive option for a sustainable energy future. Thus, it is vital to design highly active and durable electrocatalyst for OER. Herein a hybrid with the nominal composition of Ba2Co1.5Mo0.25Nb0.25O6-d (denoted as BC1.5MN) electrocatalyst consisting of both double perovskite and single perovskite structures is synthesized by a solid-state reaction method. When tested as an electrocatalyst for OER, the BC1.5MN electrocatalyst requires a current density of 10 mA cm-2 at an overpotential of 400 mV, an onset overpotential of 260 mV, and a Tafel slope of 70 mV dec-1, which are superior to that of precious metal oxide IrO2 catalyst. Chronoamperometric and cyclic voltammetry studies demonstrate that the BC1.5MN electrocatalyst has outstanding durability in alkaline solution. The synergistic effect between multi-active sites derived from a single/double perovskite hybrid structure results in one of the most active perovskite-based OER electrocatalysts in alkaline solution.
关键词： hybrid,oxygen evolution reaction,double perovskite,single perovskite,electronic structure
更新于2025-09-23 15:23:52
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Operando observation of chemical transformations of iridium oxide during photoelectrochemical water oxidation
摘要： Iridium oxide is one of the few catalysts capable of catalyzing the oxygen evolution reaction (OER) in both acidic and basic conditions. Understanding the mechanism of IrOx under realistic photoelectrochemical conditions is important for the development of integrated water splitting systems. Herein, we have developed a highly efficient OER photoanode in pH 1 aqueous solutions based on a sputtered IrOx film and a p+n-Si light absorber, interfaced with sputtered Au layer. Operando high energy resolution fluorescence detection X-ray absorption spectroscopy (HERFD XAS) was employed to monitor the oxidation state changes of IrOx during both electrochemical and photoelectrochemical (PEC) water oxidation reactions in pH 1 aqueous solutions. We observed a gradual increase of the average oxidation state of Ir with increasing anodic potential in the pre-catalytic region, followed by a reduction of Ir under O2 evolution conditions. Consistent results were obtained on dark anodes and illuminated photoanodes. However, when the thickness of IrO2 was increased to 2 and 3 nm, the spectral changes became much less pronounced and the reduction of Ir oxidation state after the OER onset was not observed. This is due to the lower surface to bulk ratio, where lattice oxygen sites in the bulk are not accessible for the formation of hydroxide. More generally, the operando method developed here can be extended to other materials, thereby providing a powerful tool for mechanism discovery and an enabling capability for catalyst design.
关键词： oxygen evolution reaction (OER),electrochemical and photoelectrochemical (PEC),high energy resolution fluorescence detection X-ray absorption spectroscopy (HERFD XAS),iridium oxide,Operando method
更新于2025-09-23 15:23:52
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Network Structured CuWO4/BiVO4/Co-Pi Nanocomposite for Solar Water Splitting
摘要： A network structured CuWO4/BiVO4 nanocomposite with a high specific surface area was prepared from CuWO4 nanoflake (NF) arrays via a method that combined drop-casting and thermal annealing. The obtained CuWO4/BiVO4 exhibited high catalytic activity toward photoelectrochemical (PEC) water oxidation. When cobalt phosphate (Co-Pi) was coupled with CuWO4/BiVO4, the activity of the resulting CuWO4/BiVO4/Co-Pi composite for the oxygen evolution reaction (OER) was further improved. The photocurrent density (Jph) for OER on CuWO4/BiVO4/Co-Pi is among the highest reported on a CuWO4-based photoanode in a neutral solution. The high activity for the PEC OER was attributed to the high specific surface area of the composite, the formation of a CuWO4/BiVO4 heterojunction that accelerated electron–hole separation, and the coupling of the Co-Pi co-catalyst with CuWO4/BiVO4, which improved the charge transfer rate across composite/solution interface.
关键词： copper tungstate,cobalt phosphate,oxygen evolution reaction,bismuth vanadate,photoelectrochemical water splitting
更新于2025-09-23 15:22:29
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Origin of the Overpotential for the Oxygen Evolution Reaction on a Well-defined Graphene Electrode Probed by in situ Sum Frequency Generation Vibrational Spectroscopy
摘要： To develop an efficient material for the cathode of the lithium-oxygen (Li-O2) secondary battery, the oxygen reduction and evolution reactions (ORR and OER) on a well-defined graphene monolayer have been investigated in a typical organic solvent, dimethyl sulfoxide (DMSO). The adsorption and desorption behaviors of the solvents on the graphene electrode surface were evaluated by an intrinsically surface-selective vibrational spectroscopy of sum frequency generation (SFG) during the ORR and OER. After the initial ORR depositing lithium peroxide (Li2O2) on the graphene electrode surface in a LiClO4/DMSO solution, the SFG spectroscopy revealed that the subsequent OER oxidizing the Li2O2 preferentially proceeds at the interface between the Li2O2 and graphene rather than that between the Li2O2 and bulk solution. Therefore, the OER tends to reduce the electric conductivity between the Li2O2 and graphene by decreasing their contact area before a large part of the deposited Li2O2 was oxidized, which elucidates the origin of the high overpotential for the OER.
关键词： oxygen reduction reaction,lithium-oxygen battery,oxygen evolution reaction,sum frequency generation vibrational spectroscopy,graphene electrode
更新于2025-09-23 15:21:01
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Spiky Nickel Electrodes for Electrochemical Oxygen Evolution Catalysis by Femtosecond Laser Structuring
摘要： Micro- and nanostructured Ni/NiO surfaces were generated by femtosecond laser structuring for oxygen evolution reaction in alkaline water electrolysis cells. For two different angles between the laser beam and the nickel surface, two different types of laser-structured electrodes were prepared, characterized, and compared with a plane tempered nickel electrode. Their electrochemical activities for the oxygen evolution reaction were tested by using cyclic and linear sweep voltammetry. The chemical surface composition was investigated by X-ray photoelectron spectroscopy. Laser structuring increased the overall electrochemical performance by more than one order of magnitude. The overpotential of the laser-structured electrodes for the oxygen evolution reaction was decreased by more than 100 mV due to high defect densities of the structures created by the laser ablation process.
关键词： nickel electrodes,femtosecond laser structuring,alkaline water electrolysis,electrochemical catalysis,oxygen evolution reaction
更新于2025-09-23 15:21:01
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Selfa??Assembled Ruddlesdena??Popper/Perovskite Hybrid with Latticea??Oxygen Activation as a Superior Oxygen Evolution Electrocatalyst
摘要： The oxygen evolution reaction (OER) is pivotal in multiple gas-involved energy conversion technologies, such as water splitting, rechargeable metal–air batteries, and CO2/N2 electrolysis. Emerging anion-redox chemistry provides exciting opportunities for boosting catalytic activity, and thus mastering lattice-oxygen activation of metal oxides and identifying the origins are crucial for the development of advanced catalysts. Here, a strategy to activate surface lattice-oxygen sites for OER catalysis via constructing a Ruddlesden–Popper/perovskite hybrid, which is prepared by a facile one-pot self-assembly method, is developed. As a proof-of-concept, the unique hybrid catalyst (RP/P-LSCF) consists of a dominated Ruddlesden–Popper phase LaSr3Co1.5Fe1.5O10-δ (RP-LSCF) and second perovskite phase La0.25Sr0.75Co0.5Fe0.5O3-δ (P-LSCF), displaying exceptional OER activity. The RP/P-LSCF achieves 10 mA cm?2 at a low overpotential of only 324 mV in 0.1 m KOH, surpassing the benchmark RuO2 and various state-of-the-art metal oxides ever reported for OER, while showing significantly higher activity and stability than single RP-LSCF oxide. The high catalytic performance for RP/P-LSCF is attributed to the strong metal–oxygen covalency and high oxygen-ion diffusion rate resulting from the phase mixture, which likely triggers the surface lattice-oxygen activation to participate in OER. The success of Ruddlesden–Popper/perovskite hybrid construction creates a new direction to design advanced catalysts for various energy applications.
关键词： electronic structure,lattice-oxygen activation,hybrid construction,oxygen evolution reaction,synergistic effects
更新于2025-09-23 15:19:57
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Remarkable Oxygen-Evolution Activity of Ca2-xSrxFe2O6-δ
摘要： The unprecedented catalytic activity of an iron-based oxygen-deficient perovskite for oxygen-evolution reaction (OER) is reported, given the need for catalysts based on earth-abundant elements. In addition, systematic trends in oxygen-evolution activity as a function of composition, defect-order and electrical conductivity have been demonstrated, leading to a methodical increase in OER catalytic activity: Ca2Fe2O6-δ < CaSrFe2O6-δ < Sr2Fe2O6-δ. The latter material, which has the highest electrical conductivity and a unique type of defect-order, exhibits the best OER activity. In conventional experiments using glassy carbon electrode, this compound shows superior OER activity compared to the current state of the art catalysts, Ba0.5Sr0.5Co0.8Fe0.2O3?δ and RuO2. It also offers an additional advantage, namely high intrinsic electrical conductivity, which allows Sr2Fe2O6-δ to act as a catalyst without the need for glassy carbon electrode or carbon powder, that are frequently used for enhancing the charge transport in OER catalysts. Indeed, pure disks of this material exhibit an outstanding activity for OER, without any additives or need for electrode preparation.
关键词： oxygen-evolution reaction,perovskite phases,iron,defect-order,electrical conductivity
更新于2025-09-23 15:19:57
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Enhancing Electrocatalytic Water Splitting Activities via Photothermal Effect over Bifunctional Nickel/Reduced Graphene Oxide Nanosheets
摘要： Electrocatalytic water splitting has huge potential for generating hydrogen fuel. Its wide application suffers from high energy loss and sluggish reaction kinetics. The adoption of appropriate electrocatalysts is capable of reducing the overpotential and accelerating the reaction. Present research mainly focuses on adjusting electrocatalysts, but the performances are also dependent on other parameters. Therefore, the development of an efficient strategy to enhance electrocatalytic performance through integrating with other driving force, especially a renewable driving force, is of great interest. Herein, we present a photothermal-effect-driven strategy to promote the electrocatalytic hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activities of nickel/reduced graphene oxide (denoted as Ni/RGO) bifunctional electrocatalysts. The Ni/RGO composite exhibited significant enhancement of activities after exposure to light irradiation (49 mV and 50 mV decrease of overpotential at 10 mA/cm2 for HER and OER, respectively). It was found that the improved electrocatalytic activities arose from the photothermal effect of Ni/RGO, which can efficiently facilitate the thermodynamics and kinetics of electrocatalytic reactions. Furthermore, the photothermal-effect-induced enhancement for electrocatalysis showed good stability, indicating its promising potential in practical application.
关键词： Bifunctional electrocatalysts,Oxygen evolution reaction,Ni/RGO nanosheets,Photothermal effect,Hydrogen evolution reaction
更新于2025-09-19 17:15:36