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

Energy & Environmental Science, Год журнала: 2023, Номер 17(1), С. 49 - 113

Опубликована: Ноя. 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.

Язык: Английский

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Electrochemical Biomass Upgrading Coupled with Hydrogen Production under Industrial‐Level Current Density

Advanced Materials, Год журнала: 2023, Номер 35(25)

Опубликована: Март 25, 2023

As promising hydrogen energy carrier, formic acid (HCOOH) plays an indispensable role in building a complete industry chain of economy. Currently, the biomass upgrading assisted water electrolysis has emerged as attractive alternative for co-producing green HCOOH and H2 cost-effective manner, yet simultaneously affording high current density Faradaic efficiency (FE) still remains big challenge. Here, ternary NiVRu-layered double hydroxides (LDHs) nanosheet arrays selective glycerol oxidation evolution catalysis are reported, which yield industry-level 1 A cm-2 at voltage 1.933 V, meanwhile showing considerable productivities 12.5 17.9 mmol h-1 , with FEs almost 80% 96%, respectively. Experimental theoretical results reveal that introduced Ru atoms can tune local electronic structure Ni-based LDHs, not only optimizes adsorption kinetics HER, but also reduces reaction barriers both conversion NiII into GOR-active NiIII carboncarbon (CC) bond cleavage. In short, this work highlights potential large-scale productions from integrated electrocatalytic system provides new insights designing advanced electrocatalyst low-cost sustainable conversion.

Язык: Английский

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A review on photo-, electro- and photoelectro- catalytic strategies for selective oxidation of alcohols

Journal of Energy Chemistry, Год журнала: 2022, Номер 77, С. 80 - 118

Опубликована: Ноя. 1, 2022

Язык: Английский

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Highly Efficient Biomass Upgrading by a Ni−Cu Electrocatalyst Featuring Passivation of Water Oxidation Activity

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(37)

Опубликована: Июль 24, 2023

Abstract Electricity‐driven organo‐oxidations have shown an increasing potential recently. However, oxygen evolution reaction (OER) is the primary competitive reaction, especially under high current densities, which leads to low Faradaic efficiency (FE) of product and catalyst detachment from electrode. Here, we report a bimetallic Ni−Cu electrocatalyst supported on Ni foam (Ni−Cu/NF) passivate OER process while oxidation 5‐hydroxymethylfurfural (HMF) significantly enhanced. A density 1000 mA cm −2 can be achieved at 1.50 V vs . reversible hydrogen electrode, both FE yield keep close 100 % over wide range potentials. Both experimental results theoretical calculations reveal that Cu doping impedes OH* deprotonation O* hereby greatly passivated. Those instructive provide new approach realizing highly efficient biomass upgrading by regulating activity.

Язык: Английский

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Electrocatalytic Refinery of Biomass-Based 5-Hydroxymethylfurfural to Fine Chemicals

ACS Catalysis, Год журнала: 2023, Номер 13(17), С. 11204 - 11231

Опубликована: Авг. 10, 2023

Because of depleting fossil-fuel reserves, together with the impacts climate change, alternative eco-friendly production high-value chemicals and renewables is needed. Biomass feedstock particular research interest. 5-Hydroxymethylfural (HMF) a versatile precursor that can be converted to via electrolysis. Reduction generates precursors for ethers, ketones, polyurethanes, polyesters, polyethers, e.g., 2,5-dihydroxymethylfuran (DHMF) 2,5-dimethyletrahydrofuran (DHMTHF), high-energy-density premium biofuels, 2,5-dimethylfuran (DMF), 2,5-hexanedione (HD) 5,5′-bis(hydroxymethyl) hydrofuroin (BHH). Oxidation HMF yields valuable chemical products, including 2,5-diformyl furan (DFF), 5-hydroxymethyl-2-furan carboxylic acid (HMFCA), 2,5-furan dicarboxylic (FDCA), maleic (MA) are precursors/intermediates polymer industry chemical/pharmaceutical production(s). In this review, we 1) report comparative summary electrocatalytic refinery HMF, both electro-oxidation electroreduction pathways, 2) appraise advances in reaction (HRR) (HOR), 3) assess pathways mechanisms, 4) establish design electrocatalysts selection metal materials, geometric structure, electronic structural modifications boost HRR HOR activity selectivity, 5) evaluate impact parameters pH, electrolyte composition, applied potential, initial substrate concentration on HOR, 6) provide prospect future electrochemical refinement HMF. We conclude an improved understanding conditions needed practically selectivity Findings will benefit electrochemistry chemistry generating fine and, therefore, interest researchers manufacturers.

Язык: Английский

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In Situ Immobilizing Atomically Dispersed Ru on Oxygen-Defective Co₃O₄ for Efficient Oxygen Evolution

ACS Catalysis, Год журнала: 2023, Номер 13(4), С. 2462 - 2471

Опубликована: Фев. 2, 2023

The synergistic regulation of the electronic structures transition-metal oxide-based catalysts via oxygen vacancy defects and single-atom doping is efficient to boost their evolution reaction (OER) performance, which remains challenging due complex synthetic procedures. Herein, a facile defect-induced in situ deposition strategy developed anchor atomically dispersed Ru onto vacancy-rich cobalt oxides (Ru/Co3O4–x) based on spontaneous redox between Ru3+ ions nonstoichiometric Co3O4–x. Accordingly, as-prepared Ru/Co3O4–x electrocatalyst with coexistence vacancies atoms exhibits excellent performances toward OER low overpotential 280 mV at 10 mA cm–2, small Tafel slope value 86.9 dec–1, good long-term stability alkaline media. Furthermore, density functional theory calculations uncover that could synergistically tailor electron decentralization d-band center Co atoms, further optimizing adsorption oxygen-based intermediates (*OH, *O, *OOH) reducing barriers OER. This work proposes an available for constructing electrocatalysts abundant noble metal presents deep understanding engineering transition-metal-based evolution.

Язык: Английский

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Ambient Electrosynthesis toward Single‐Atom Sites for Electrocatalytic Green Hydrogen Cycling

Advanced Materials, Год журнала: 2023, Номер 35(14)

Опубликована: Фев. 17, 2023

With the ultimate atomic utilization, well-defined configuration of active sites and unique electronic properties, catalysts with single-atom (SASs) exhibit appealing performance for electrocatalytic green hydrogen generation from water splitting further utilization via hydrogen-oxygen fuel cells, such that a vast majority synthetic strategies toward SAS-based (SASCs) are exploited. In particular, room-temperature electrosynthesis under atmospheric pressure offers novel, safe, effective route to access SASs. Herein, recent progress in ambient SASs sustainable future opportunities discussed. A systematic summary is started on three kinds electrochemically routes SASs, including electrochemical etching (ECE), direct electrodeposition (DED), leaching-redeposition (ELR), associated advanced characterization techniques. Next, their applications energy conversion evolution reaction, oxygen overall splitting, reduction reaction reviewed. Finally, brief conclusion remarks challenges regarding development high-performance cost-effective SASCs many other presented.

Язык: Английский

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Emerging Xene‐Based Single‐Atom Catalysts: Theory, Synthesis, and Catalytic Applications

Advanced Materials, Год журнала: 2023, Номер 36(3)

Опубликована: Июнь 17, 2023

Abstract In recent years, the emergence of novel 2D monoelemental materials (Xenes), e.g., graphdiyne, borophene, phosphorene, antimonene, bismuthene, and stanene, has exhibited unprecedented potentials for their versatile applications as well addressing new discoveries in fundamental science. Owing to unique physicochemical, optical, electronic properties, emerging Xenes have been regarded promising candidates community single‐atom catalysts (SACs) active sites or support matrixes significant improvement intrinsic activity selectivity. order comprehensively understand relationships between structure property Xene‐based SACs, this review represents a comprehensive summary from theoretical predictions experimental investigations. Firstly, calculations regarding both anchoring on doping/substituting heteroatoms at are briefly summarized. Secondly, controlled synthesis precise characterization presented SACs. Finally, current challenges future opportunities development SACs highlighted.

Язык: Английский

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Pulse potential mediated selectivity for the electrocatalytic oxidation of glycerol to glyceric acid

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Март 18, 2024

Abstract Preventing the deactivation of noble metal-based catalysts due to self-oxidation and poisonous adsorption is a significant challenge in organic electro-oxidation. In this study, we employ pulsed potential electrolysis strategy for selective electrocatalytic oxidation glycerol glyceric acid over Pt-based catalyst. situ Fourier-transform infrared spectroscopy, quasi-in X-ray photoelectron finite element simulations reveal that could tailor catalyst’s surface micro-environment. This prevents overaccumulation poisoning intermediate species frees up active sites re-adsorption OH adsorbate glycerol. The results higher selectivity (81.8%) than constant-potential electrocatalysis with 0.7 V RHE (37.8%). work offers an efficient mitigate electrocatalysts.

Язык: Английский

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Controllable Electron Distribution Reconstruction of Spinel NiCo₂O₄ Boosting Glycerol Oxidation at Elevated Current Density

Advanced Functional Materials, Год журнала: 2023, Номер 34(3)

Опубликована: Окт. 5, 2023

Abstract Electrocatalytic glycerol oxidation reaction (GOR) is an effective way to convert biomass byproduct high value‐added chemicals, which; however, suffers from the low activity and conversion ratio of presently available catalysts. Herein, NiCo 2 O 4 /NF bimetallic oxide nanoarray controllably fabricated by Ni substituting for octahedral Co 3+ in 3 , which exhibits excellent GOR catalytic at elevated current densities ( E 300 = 1.42 V, 600 1.62 V) overall Faradaic efficiency 97.5% V (FE formic acid 89.9% FE glycolic 7.62%). The performance attributed structure evolution including rapid generation III ‐OOH active species, optimized intermediates adsorption, accelerated electron transfer owing introduction, are evidenced operando spectroscopy measurements density functional theory calculations, respectively. GOR/hydrogen coupled two‐electrode electrolytic cell voltage ≈299 mV lower than that water splitting 50 mA cm −2 . More importantly, compared conventional splitting, this electrolyzer stable over 200 h 1.75 reducing energy consumption 16.9% obtaining products anode concurrently.

Язык: Английский

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