Bifunctional Electrocatalysts for Overall and Hybrid Water Splitting

Chemical Reviews, Год журнала: 2024, Номер 124(7), С. 3694 - 3812

Опубликована: Март 22, 2024

Electrocatalytic water splitting driven by renewable electricity has been recognized as a promising approach for green hydrogen production. Different from conventional strategies in developing electrocatalysts the two half-reactions of (e.g., and oxygen evolution reactions, HER OER) separately, there growing interest designing bifunctional electrocatalysts, which are able to catalyze both OER. In addition, considering high overpotentials required OER while limited value produced oxygen, is another rapidly exploring alternative oxidation reactions replace hybrid toward energy-efficient generation. This Review begins with an introduction on fundamental aspects splitting, followed thorough discussion various physicochemical characterization techniques that frequently employed probing active sites, emphasis reconstruction during redox electrolysis. The design, synthesis, performance diverse based noble metals, nonprecious metal-free nanocarbons, overall acidic alkaline electrolytes, thoroughly summarized compared. Next, their application also presented, wherein anodic include sacrificing agents oxidation, pollutants oxidative degradation, organics upgrading. Finally, concise statement current challenges future opportunities presented hope guiding endeavors quest sustainable

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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Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Сен. 20, 2023

Renewable energy-based electrocatalytic oxidation of organic nucleophiles (e.g.methanol, urea, and amine) are more thermodynamically favourable and, economically attractive to replace conventional pure water electrooxidation in electrolyser produce hydrogen. However, it is challenging due the competitive oxygen evolution reaction under a high current density (e.g., >300 mA cm-2), which reduces anode electrocatalyst's activity stability. Herein, taking lower energy cost urea as model reaction, we developed oxyanion-engineered Nickel catalysts inhibit competing during achieving an ultrahigh 323.4 cm-2 at 1.65 V with 99.3 ± 0.4% selectivity N-products. In situ spectra studies reveal that such generated oxyanions not only OH- adsorption guarantee coverage reactant on active sites avoid but also accelerate urea's C - N bond cleavage form CNO intermediates for facilitating reaction. Accordingly, comprehensive mechanism behaviour between boost dynamic change Ni was proposed. This work presents feasible route high-efficiency even various reactions practical applications.

Язык: Английский

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Doped Mn Enhanced NiS Electrooxidation Performance of HMF into FDCA at Industrial‐Level Current Density

Advanced Functional Materials, Год журнала: 2023, Номер 33(24)

Опубликована: Март 13, 2023

Abstract Electrooxidation of 5‐hydroxymethylfurfural (HMF) into 2,5‐furandicarboxylic acid (FDCA) is a highly promising approach for producing value‐added chemicals from biomass. However, developing efficient electrocatalysts HMF oxidation (HMFOR) with high current density in large‐scale productions remains challenge. Herein, it demonstrated that the Mn‐doped NiS nanosheet grown directly on 3D graphite felt (GF) substrates can efficiently perform electrooxidation FDCA at industrial‐level (500 mA cm −2 ) H‐cell. The Mn 0.2 NiS/GF exhibits excellent HMFOR performance selectivity (98.3%), yield (97.6%), faradaic efficiency (94.2%), and robust stability (10 cycles). Especially, production rate up to 4.56 g h −1 be achieved, superior those reported literatures. Furthermore, by scaling electrode area assembling continuous‐flow electrolyzer, 44.32 achieved. activity attributed incorporation material, theoretical calculation results indicate Ni as both adsorption sites oxidation, thereby effectively facilitate electro‐oxidation performance. This work provides strategy potential industrial‐grade large density.

Язык: Английский

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Concerted and Selective Electrooxidation of Polyethylene‐Terephthalate‐Derived Alcohol to Glycolic Acid at an Industry‐Level Current Density over a Pd−Ni(OH)₂ Catalyst

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(11)

Опубликована: Янв. 19, 2023

Electro-reforming of Polyethylene-terephthalate-derived (PET-derived) ethylene glycol (EG) into fine chemicals and H2 is an ideal solution to address severe plastic pollution. Here, we report the electrooxidation EG glycolic acid (GA) with a high Faraday efficiency selectivity (>85 %) even at industry-level current density (600 mA cm-2 1.15 V vs. RHE) over Pd-Ni(OH)2 catalyst. Notably, stable electrolysis 200 h can be achieved, outperforming all available Pd-based catalysts. Combined experimental theoretical results reveal that 1) OH* generation promoted by Ni(OH)2 plays critical role in facilitating EG-to-GA oxidation removing poisonous carbonyl species, thereby achieving activity stability; 2) Pd downshifted d-band center oxophilic Ni synergistically facilitate rapid desorption transfer GA from active sites inactive sites, avoiding over-oxidation thus selectivity.

Язык: Английский

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Recent Advancements in Electrochemical Hydrogen Production via Hybrid Water Splitting

Advanced Materials, Год журнала: 2023, Номер 36(4)

Опубликована: Окт. 10, 2023

Abstract As one of the most promising approaches to producing high‐purity hydrogen (H 2 ), electrochemical water splitting powered by renewable energy sources such as solar, wind, and hydroelectric power has attracted considerable interest over past decade. However, electrolysis process is seriously hampered sluggish electrode reaction kinetics, especially four‐electron oxygen evolution at anode side, which induces a high overpotential. Currently, emerging hybrid strategy proposed integrating thermodynamically favorable electro–oxidation reactions with cathode, providing new opportunity for energy–efficient H2 production. To achieve highly efficient cost–effective toward large–scale practical H production, much work been continuously done exploit alternative anodic oxidation cutting–edge electrocatalysts. This review will focus on recent developments production coupled reactions, including choice substrates, investigation electrocatalytic materials, deep understanding underlying mechanisms. Finally, some insights into scientific challenges now standing in way future advancement technique are shared, hope inspiring further innovative efforts this rapidly growing field.

Язык: Английский

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Collaborative Interface Optimization Strategy Guided Ultrafine RuCo and MXene Heterostructure Electrocatalysts for Efficient Overall Water Splitting

ACS Nano, Год журнала: 2023, Номер 17(11), С. 10947 - 10957

Опубликована: Май 18, 2023

Developing highly active and robust electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER) is crucial large-scale utilization of green hydrogen. In this study, a collaborative interface optimization guided strategy was employed to prepare metal-organic framework (MOF) derived heterostructure electrocatalyst (MXene@RuCo NPs). The obtained requires overpotentials only 20 mV HER 253 OER deliver current density 10 mA/cm2 in alkaline media, respectively, it also exhibits great performance at high density. Experiments theoretical calculations reveal that doped Ru introduces second sites decreases diameter nanoparticles, which greatly enhances number sites. More importantly, MXene/RuCo NPs heterogeneous interfaces catalysts exhibit synergistic effects, decreasing work function catalyst improving charge transfer rate, thus reducing energy barrier catalytic reaction. This represents promising development MOF-derived achieve efficient conversion industrial applications.

Язык: Английский

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Recent Advances on Transition‐Metal‐Based Layered Double Hydroxides Nanosheets for Electrocatalytic Energy Conversion

Advanced Science, Год журнала: 2023, Номер 10(13)

Опубликована: Март 3, 2023

Abstract Transition‐metal‐based layered double hydroxides (TM‐LDHs) nanosheets are promising electrocatalysts in the renewable electrochemical energy conversion system, which regarded as alternatives to noble metal‐based materials. In this review, recent advances on effective and facile strategies rationally design TM‐LDHs electrocatalysts, such increasing number of active sties, improving utilization sites (atomic‐scale catalysts), modulating electron configurations, controlling lattice facets, summarized compared. Then, these fabricated for oxygen evolution reaction, hydrogen urea oxidation nitrogen reduction small molecule oxidations, biomass derivatives upgrading is articulated through systematically discussing corresponding fundamental principles reaction mechanism. Finally, existing challenges density catalytically future prospects nanosheets‐based each application also commented.

Язык: Английский

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Advances in Selective Electrochemical Oxidation of 5‐Hydroxymethylfurfural to Produce High‐Value Chemicals

Advanced Science, Год журнала: 2022, Номер 10(4)

Опубликована: Дек. 8, 2022

The conversion of biomass is a favorable alternative to the fossil energy route solve crisis and environmental pollution. As one most versatile platform compounds, 5-hydroxymethylfural (HMF) can be transformed various value-added chemicals via electrolysis combining with renewable energy. Here, recent advances in electrochemical oxidation HMF, from reaction mechanism reactor design are reviewed. First, pathway summarized systematically. Second, parameters easy ignored emphasized discussed. Then, electrocatalysts reviewed comprehensively for different products reactors introduced. Finally, future efforts on exploring mechanism, electrocatalysts, prospected. This review provides deeper understanding electrocatalyst reactor, which expected promote economical efficient industrial applications.

Язык: Английский

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Intermetallic Nanocrystals for Fuel-Cells-Based Electrocatalysis

Chemical Reviews, Год журнала: 2023, Номер 123(22), С. 12507 - 12593

Опубликована: Ноя. 1, 2023

Electrocatalysis underpins the renewable electrochemical conversions for sustainability, which further replies on metallic nanocrystals as vital electrocatalysts. Intermetallic have been known to show distinct properties compared their disordered counterparts, and long explored functional improvements. Tremendous progresses made in past few years, with notable trend of more precise engineering down an atomic level investigation transferring into practical membrane electrode assembly (MEA), motivates this timely review. After addressing basic thermodynamic kinetic fundamentals, we discuss classic latest synthetic strategies that enable not only formation intermetallic phase but also rational control other catalysis-determinant structural parameters, such size morphology. We demonstrate emerging nanomaterials potentially advancement energy electrocatalysis. Then, state-of-the-art characterizations representative electrocatalysts emphasis oxygen reduction reaction evaluated a MEA setup. summarize review by laying out existing challenges offering perspective future research directions toward practicing conversions.

Язык: Английский

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