Recent Advances in Design of Electrocatalysts for High‐Current‐Density Water Splitting

Advanced Materials, Год журнала: 2021, Номер 34(16)

Опубликована: Дек. 4, 2021

Abstract Electrochemical water splitting technology for producing “green hydrogen” is important the global mission of carbon neutrality. Electrocatalysts with decent performance at high current densities play a central role in industrial implementation this technology. This field has advanced immensely recent years, as witnessed by many types catalysts designed and synthesized toward industriallyrelevant (>200 mA cm –2 ). By discussing advances field, several key aspects are summarized that affect catalytic high‐current‐density electrocatalysis, including dimensionality catalysts, surface chemistry, electron transport path, morphology, catalyst‐electrolyte interplay. The multiscale design strategy considers these comprehensively developing electrocatalysts highlighted. perspectives on future directions emerging also put forward.

Язык: Английский

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Synergistic effect of multiple vacancies to induce lattice oxygen redox in NiFe-layered double hydroxide OER catalysts

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 323, С. 122091 - 122091

Опубликована: Ноя. 3, 2022

Язык: Английский

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Transition metal-based catalysts for electrochemical water splitting at high current density: current status and perspectives

Nanoscale, Год журнала: 2021, Номер 13(30), С. 12788 - 12817

Опубликована: Янв. 1, 2021

Current popular transition metal-based electrocatalysts developed for HER/OER in water splitting at high current density are critically reviewed and discussed.

Язык: Английский

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Accelerating CO₂ Electroreduction to Multicarbon Products via Synergistic Electric–Thermal Field on Copper Nanoneedles

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(7), С. 3039 - 3049

Опубликована: Фев. 3, 2022

Electrochemical CO2 reduction is a promising way to mitigate emissions and close the anthropogenic carbon cycle. Among products from CO2RR, multicarbon chemicals, such as ethylene ethanol with high energy density, are more valuable. However, selectivity reaction rate of C2 production unsatisfactory due sluggish thermodynamics kinetics C-C coupling. The electric field thermal have been studied utilized promote catalytic reactions, they can regulate thermodynamic kinetic barriers reactions. Either raising potential or heating electrolyte enhance coupling, but these come at cost increasing side hydrogen evolution reaction. Here, we present generic strategy local temperature simultaneously dramatically improve electric-thermal synergy desired in electrocatalysis. A conformal coating ∼5 nm polytetrafluoroethylene significantly improves ability copper nanoneedles (∼7-fold ∼40 K enhancement tips compared bare experimentally), resulting an improved Faradaic efficiency over 86% partial current density than 250 mA cm-2 record-high turnover frequency 11.5 ± 0.3 s-1 Cu site-1. Combined its low scalability, for state-of-the-art catalyst not only offers new insight into improving activity value-added demonstrated also inspires advances and/or other valuable electro-/photocatalysis evolution, nitrogen reduction, peroxide electrosynthesis.

Язык: Английский

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Triggering Lattice Oxygen Activation of Single‐Atomic Mo Sites Anchored on Ni–Fe Oxyhydroxides Nanoarrays for Electrochemical Water Oxidation

Advanced Materials, Год журнала: 2022, Номер 34(29)

Опубликована: Май 17, 2022

Tuning the reactivity of lattice oxygen is significance for lowering energy barriers and accelerating evolution reaction (OER). Herein, single-atomic Mo sites are anchored on Ni-Fe oxyhydroxide nanoarrays by a facile metal-organic-framework-derived strategy, exhibiting superior performance toward OER in alkaline media. In situ electrochemical spectroscopy isotope-labeling experiments reveal involvement during cycles. Combining theoretical experimental investigations electronic configuration, it comprehensively confirmed that incorporation enables higher oxidation state metal strengthened metal-oxygen hybridization, as well formation oxidized ligand holes above Fermi level. word, considerable acceleration water achieved via enhancing triggering activation. This work may provide new insights designing ideal electrocatalysts tuning chemical activating anions ligands.

Язык: Английский

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Ion Sieve: Tailoring Zn²⁺ Desolvation Kinetics and Flux toward Dendrite-Free Metallic Zinc Anodes

ACS Nano, Год журнала: 2021, Номер 16(1), С. 1013 - 1024

Опубликована: Дек. 17, 2021

Tip-induced dendrites on metallic zinc anodes (MZAs) fundamentally deteriorate the rechargeability of aqueous Zn metal batteries (ZMBs). Herein, an intriguing ion sieve (IS) consisting 3D intertwined bacterial cellulose, deposited surface MZAs (Zn@IS) through in situ self-assembly route, is first presented to be effective inhibiting dendrite-growth MZAs. Experimental analyses together with theoretical calculations suggested that IS coating can facilitate desolvation [Zn(H2O)6]2+ clusters via a strong interplay ions, weaken hydrogen evolution reaction MZAs, and homogenize flux abundant nanopores serving as tunnels, synergistically enabling dendrite-free deposition Zn@IS anodes. Consequently, lifespan up 3000 h at cutoff capacity 0.25 mA cm–2 was observed Zn@IS∥Zn@IS symmetric cell. In terms application, pairing carbon-nanotube@MnO2 cathode example, full ZMBs acquired enhanced much higher retention over 73.3% after cycles compared counterpart pristine MZA (21%).

Язык: Английский

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Highly Curved Nanostructure‐Coated Co, N‐Doped Carbon Materials for Oxygen Electrocatalysis

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(23), С. 12759 - 12764

Опубликована: Март 1, 2021

Abstract Nitrogen‐doped graphene could catalyze the electrochemical reduction and evolution of oxygen, but unfortunately suffers from sluggish catalytic kinetics. Herein, for first time, we report an onion‐like carbon coated Co, N‐doped (OLC/Co‐N‐C) material, which possesses multilayers highly curved nanostructures that form mesoporous architectures. These unique nanospheres are produced when surfactant micelles introduced to synthesis precursors. Owing combined electronic effect nanostructuring effect, our OLC/Co‐N‐C materials exhibit high bifunctional oxygen reduction/evolution reaction (ORR/OER) activity, showing a promising application in rechargeable Zn‐air batteries. Experimental results rationalized by theoretical calculations, curvature graphitic plays vital role promoting activities meta‐carbon atoms near N ortho/meta close pyridinic N.

Язык: Английский

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Improved Interface Charge Transfer and Redistribution in CuO‐CoOOH p‐n Heterojunction Nanoarray Electrocatalyst for Enhanced Oxygen Evolution Reaction

Advanced Science, Год журнала: 2021, Номер 8(22)

Опубликована: Окт. 12, 2021

Abstract Electron density modulation is of great importance in an attempt to achieve highly active electrocatalysts for the oxygen evolution reaction (OER). Here, successful construction CuO@CoOOH p‐n heterojunction (i.e., p‐type CuO and n‐type CoOOH) nanoarray electrocatalyst through situ anodic oxidation CuO@CoS x on copper foam reported. The can remarkably modify electronic properties space‐charge region facilitate electron transfer. Moreover, Raman study reveals generation SO 4 2− from CoS oxidation, cloud distribution functional theory calculation suggest that surface‐adsorbed OER process by enhancing adsorption OH − . positively charged CoOOH significantly enhance activity. As a result, shows enhanced performance with low overpotential 186 mV afford current 10 mA cm −2 preparation large scale (14 × 25 2 ) sample demonstrates possibility promoting catalyst industrial‐scale production. This offers new insights into design fabrication non‐noble metal‐based as effective catalytic materials energy storage conversion.

Язык: Английский

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Operando spectroscopies unveil interfacial FeOOH induced highly reactive β-Ni(Fe)OOH for efficient oxygen evolution

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 318, С. 121825 - 121825

Опубликована: Авг. 8, 2022

Язык: Английский

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Engineering Metallic Heterostructure Based on Ni₃N and 2M‐MoS₂ for Alkaline Water Electrolysis with Industry‐Compatible Current Density and Stability

Advanced Materials, Год журнала: 2021, Номер 34(9)

Опубликована: Дек. 30, 2021

Alkaline water electrolysis is commercially desirable to realize large-scale hydrogen production. Although nonprecious catalysts exhibit high electrocatalytic activity at low current density (10-50 mA cm-2 ), it still challenging achieve industrially required over 500 due inefficient electron transport and competitive adsorption between hydroxyl water. Herein, the authors design a novel metallic heterostructure based on nickel nitride monoclinic molybdenum disulfide (Ni3 N@2M-MoS2 ) for extraordinary electrolysis. The Ni3 composite with heterointerface provides two kinds of separated reaction sites overcome steric hindrance hydroxyl/water adsorption. kinetically decoupled adsorption/dissociation conductivity enable production from N oxygen evolution large density. proved be imperative stabilization activation , which can efficiently regulate active electronic states Ni/N atoms around Fermi-level through charge transfer MoMo bonds 2M-MoS2 boost overall splitting. incorporated electrolyzer requires ultralow cell voltage 1.644 V@1000 ≈100% retention 300 h, far exceeding commercial Pt/C║RuO2 (2.41 100 58.2%).

Язык: Английский

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