Progress in Hydrogen Production Coupled with Electrochemical Oxidation of Small Molecules

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(51)

Published: Oct. 6, 2022

Abstract The electrochemical oxidation of small molecules to generate value‐added products has gained enormous interest in recent years because the advantages benign operation conditions, high conversion efficiency and selectivity, absence external oxidizing agents, eco‐friendliness. Coupling replace oxygen evolution reaction (OER) at anode hydrogen (HER) cathode an electrolyzer would simultaneously realize generation high‐value chemicals or pollutant degradation highly efficient production hydrogen. This Minireview presents introduction on small‐molecule choice design strategies electrocatalysts as well breakthroughs achieved Finally, challenges future orientations are highlighted.

Language: Английский

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Rapid complete reconfiguration induced actual active species for industrial hydrogen evolution reaction

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Oct. 2, 2022

Rational regulation of electrochemical reconfiguration and exploration activity origin are important foundations for realizing the optimization electrocatalyst activity, but rather challenging. Herein, we potentially develop a rapid complete strategy heterostructures CoC2O4 coated by MXene nanosheets (CoC2O4@MXene) during hydrogen evolution reaction (HER) process. The self-assembled CoC2O4@MXene nanotubular structure has high electronic accessibility abundant electrolyte diffusion channels, which favor reconfiguration. Such creates new actual catalytic active species Co(OH)2 transformed from CoC2O4, is coupled with to facilitate charge transfer decrease free energy Volmer step toward fast HER kinetics. reconfigured components require low overpotentials 28 216 mV at 10 1000 mA cm-2 in alkaline conditions decent stability natural seawater. This work gives insights understanding formation opens up way high-performance electrocatalysts.

Language: Английский

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Phosphated IrMo bimetallic cluster for efficient hydrogen evolution reaction

eScience, Journal Year: 2022, Volume and Issue: 2(3), P. 304 - 310

Published: April 15, 2022

Developing low-cost, high-performance electrocatalysts for the hydrogen evolution reaction (HER) is essential producing from renewable energy sources. Herein, we report phosphated IrMo bimetallic clusters supported by macroporous nitrogen-doped carbon (IrMoP/MNC) as a highly efficient alkaline HER catalyst. The experimental and theoretical results demonstrate that P Mo synergistically tune electronic structure of atomically dispersed Ir to improve adsorption reactant H2O desorption product OH−. itself serves an active site cooperates with nearby atom significantly enhance kinetics. Even only 2.6 ​wt% in catalyst, IrMoP/MNC exhibits ultralow overpotential 14 ​mV at 10 ​mA ​cm−2, well unprecedented high mass activity 18.58 A mgIr−1 100 ​mV, superior commercial Pt/C overwhelmingly better than other Ir-based electrocatalysts. This study demonstrates multi-level design strategy effectively efficiency noble metal, involving spatial geometry, local structure, dual-atom synergy.

Language: Английский

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Lattice‐Matching Formed Mesoporous Transition Metal Oxide Heterostructures Advance Water Splitting by Active Fe–O–Cu Bridges

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(19)

Published: April 8, 2022

Abstract Developing efficient bifunctional electrocatalysts toward oxygen/hydrogen evolution reactions is crucial for electrochemical water splitting hydrogen production. The high‐performance depend on the catalytically active and highly accessible reaction sites their structural robustness, while rational design of such with desired features avoiding tedious manufacture still challenging. Here, a facile method reported to synthesize mesoporous heterostructured transition metal oxides strongly anchored nickel skeleton (MH‐TMO) containing identified Fe–Cu oxide interfaces high intrinsic activity, easy accessibility intermediates, long‐term stability alkaline reactions. MH‐TMO electrocatalytically Fe–O–Cu bridge has an optimal oxygen binding energy facilitate adsorption/desorption intermediates molecules. Associated mass transport through nanoporous structure, exhibits impressive catalysis, extremely low overpotential around 0.22 V at 10 mA cm −2 Tafel slope (44.5 mV dec −1 ) in 1.0 M KOH, realizing current density 100 as 0.26 V. As result, electrolyzer assembled by catalysts operates outstanding overall water‐splitting output (1.49 V@10 ), outperforming one noble‐metal‐based catalysts.

Language: Английский

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Highly Active and Durable Single‐Atom Tungsten‐Doped NiS_0.5Se_0.5 Nanosheet @ NiS_0.5Se_0.5 Nanorod Heterostructures for Water Splitting

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(13)

Published: Jan. 26, 2022

Developing robust and highly active non-precious electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER) is crucial industrialization of hydrogen energy. In this study, a durable single-atom W-doped NiS0.5 Se0.5 nanosheet @ nanorod heterostructure (W-NiS0.5 ) electrocatalyst prepared. W-NiS0.5 exhibits excellent catalytic activity HER OER with ultralow overpotentials (39 106 mV 171 239 at 10 100 mA cm-2 , respectively) long-term durability (500 h), outperforming commercial precious-metal catalysts many other previously reported transition-metal-based compounds (TMCs). The introduction W delocalizes spin state Ni, which results in an increase Ni d-electron density. This causes optimization adsorption/desorption process H significant reduction adsorption free energy rate-determining step (O* → OOH*), thus accelerating thermodynamics kinetics OER. work provides rational feasible strategy to design water splitting develop advanced TMC by regulating delocalized states.

Language: Английский

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Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(1), P. 49 - 113

Published: Nov. 7, 2023

This perspective highlights recent advancements in innovative strategies to provide valuable insights into the potential for energy-saving hydrogen production through water electrolysis.

Language: Английский

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PEM water electrolysis for hydrogen production: fundamentals, advances, and prospects

Carbon Neutrality, Journal Year: 2022, Volume and Issue: 1(1)

Published: June 2, 2022

Hydrogen, as a clean energy carrier, is of great potential to be an alternative fuel in the future. Proton exchange membrane (PEM) water electrolysis hailed most desired technology for high purity hydrogen production and self-consistent with volatility renewable energies, has ignited much attention past decades based on current density, greater efficiency, small mass-volume characteristic, easy handling maintenance. To date, substantial efforts have been devoted development advanced electrocatalysts improve electrolytic efficiency reduce cost PEM electrolyser. In this review, we firstly compare alkaline (AWE), solid oxide (SOE), highlight advantages electrolysis. Furthermore, summarize recent progress including evolution reaction (HER) oxygen (OER) acidic electrolyte. We also introduce other cell components (including electrode assembly, collector, bipolar plate). Finally, challenges outlook future application are provided.

Language: Английский

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Single atomic cobalt electrocatalyst for efficient oxygen reduction reaction

eScience, Journal Year: 2022, Volume and Issue: 2(4), P. 399 - 404

Published: May 18, 2022

Robust oxygen reduction reaction (ORR) catalysts are essential for energy storage and conversion devices, but their development remains challenging. Herein, we design a single-atom catalyst featuring isolated Co anchored on nitrogen-doped carbon (Co-SAC/NC) via highly efficient “plasma-bombing” strategy. With high loading (up to 2.5 ​wt%), the well-dispersed single atoms in Co-SAC/NC give it robust ORR performance an alkaline medium. It also demonstrates excellent battery when implemented as air-cathode zinc-air (ZAB). Theoretical calculations reveal that Co–N4 moiety experiences “extraction/recovery” structural evolution during process, reaction's rate-determining step is formation of OOH∗ (reaction intermediate). This work provides new strategy designing high-performance ZABs other energy-conversion devices.

Language: Английский

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Interfacial Engineering of Ni₃N/Mo₂N Heterojunctions for Urea-Assisted Hydrogen Evolution Reaction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(7), P. 4091 - 4100

Published: March 9, 2023

The urea oxidation reaction (UOR) is considered as an alternative to the oxygen evolution for high-efficiency hydrogen production. However, molecule relatively complex, containing both electron-donating amino (−NH2) and electron-withdrawing carbonyl (C═O) groups, understanding influence of different functional groups on adsorption behavior conducive rational design preparation high-performance UOR catalysts. Herein, we report a simple synthesis Ni3N/Mo2N heterostructure systematic investigation urea-assisted electrolytic Both temperature-programmed desorption theoretical calculations decipher that −NH2 C═O are more easily adsorbed Ni3N Mo2N, respectively. Meanwhile, could combine enhance advantages individual components, optimizing urea. Besides, this also beneficial improving performance. As expected, in two-electrode water electrolyzer utilizing bifunctional catalysts, production can readily occur at evidently lower voltage (1.36 V@10 mA cm–2), which much than traditional electrolysis, well 7 times higher rate achieved.

Language: Английский

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Synergistic Engineering of Doping and Vacancy in Ni(OH)₂ to Boost Urea Electrooxidation

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(4)

Published: Nov. 16, 2022

Abstract Nickel hydroxide (Ni(OH) 2 ) has been identified as one of the best promising electrocatalyst candidates for urea oxidation reaction (UOR) due to its flexible structures, wide compositions, and abundant 3d electrons under alkaline conditions. However, layered structure with limited exposed edge sites severely hinders further improvement UOR activity. Herein, oxygen‐vacancy rich vanadium doped Ni(OH) (O vac ‐V‐Ni(OH) catalysts are prepared synergistically boost electrooxidation. Vanadium doping contributes more active sites, simultaneously generates oxygen vacancies, switching rate‐determining step from *COOH deprotonation N–H bond cleavage process lowering thermodynamic barrier by around 1.13 eV. The novel O demonstrates good electrocatalytic performances a working potential 1.47 V at high current density 100 mA cm −2 . Synergistic engineering vacancy is strategy designing efficient electrocatalysts.

Language: Английский

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