Clean and Affordable Hydrogen Fuel from Alkaline Water Splitting: Past, Recent Progress, and Future Prospects

Advanced Materials, Год журнала: 2021, Номер 33(31)

Опубликована: Июнь 12, 2021

Abstract Hydrogen economy has emerged as a very promising alternative to the current hydrocarbon economy, which involves process of harvesting renewable energy split water into hydrogen and oxygen then further utilization clean fuel. The production by electrolysis is an essential prerequisite with zero carbon emission. Among various technologies, alkaline splitting been commercialized for more than 100 years, representing most mature economic technology. Here, historic development overviewed, several critical electrochemical parameters are discussed. After that, advanced nonprecious metal electrocatalysts that recently negotiating evolution reaction (OER) (HER) discussed, including transition oxides, (oxy)hydroxides, chalcogenides, phosphides, nitrides OER, well alloys, carbides HER. In this section, particular attention paid catalyst synthesis, activity stability challenges, performance improvement, industry‐relevant developments. Some recent works about scaled‐up novel electrode designs, seawater also spotlighted. Finally, outlook on future challenges opportunities offered, potential directions speculated.

Язык: Английский

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Interfacial Engineering of MoO₂‐FeP Heterojunction for Highly Efficient Hydrogen Evolution Coupled with Biomass Electrooxidation

Advanced Materials, Год журнала: 2020, Номер 32(17)

Опубликована: Март 16, 2020

Abstract Simultaneous highly efficient production of hydrogen and conversion biomass into value‐added products is meaningful but challenging. Herein, a porous nanospindle composed carbon‐encapsulated MoO 2 ‐FeP heterojunction (MoO ‐FeP@C) proposed as robust bifunctional electrocatalyst for evolution reaction (HER) electrooxidation (BEOR). X‐ray photoelectron spectroscopy analysis theoretical calculations confirm the electron transfer from to FeP at interfaces, where accumulation on favors optimization H O H* absorption energies HER, whereas hole responsible improving BEOR activity. Thanks its interfacial electronic structure, ‐FeP@C exhibits excellent HER activity with an overpotential 103 mV 10 mA cm −2 Tafel slope 48 dec −1 . Meanwhile, when 5‐hydroxymethylfurfural chosen BEOR, almost 100%, 2,5‐furandicarboxylic acid (FDCA) obtained selectivity 98.6%. The electrolyzer employing cathodic anodic FDCA requires only low voltage 1.486 V can be powered by solar cell (output voltage: 1.45 V). Additionally, other BEORs coupled catalyzed also have catalytic performance, implying their good versatility.

Язык: Английский

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Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(36), С. 19572 - 19590

Опубликована: Фев. 19, 2021

Abstract Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy convert renewable feedstocks energy sources into transportable fuels value‐added chemicals. A crucial step in conducting e‐refinery processes development of appropriate reactions optimal electrocatalysts for efficient cleavage formation chemical bonds. However, compared well‐studied primary (e.g., O 2 reduction, water splitting), mechanistic aspects materials design complex are yet be settled. To address this challenge, herein, we first present fundamentals heterogeneous electrocatalysis some reactions, then implement these establish framework by coupling situ generated intermediates (integrated reactions) or products (tandem reactions). We also set principles strategies efficiently manipulate reaction pathways.

Язык: Английский

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Activity Origins and Design Principles of Nickel-Based Catalysts for Nucleophile Electrooxidation

Chem, Год журнала: 2020, Номер 6(11), С. 2974 - 2993

Опубликована: Авг. 18, 2020

Язык: Английский

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Unveiling the Electrooxidation of Urea: Intramolecular Coupling of the N−N Bond

Angewandte Chemie International Edition, Год журнала: 2020, Номер 60(13), С. 7297 - 7307

Опубликована: Дек. 25, 2020

Abstract The nitrogenous nucleophile electrooxidation reaction (NOR) plays a vital role in the degradation and transformation of available nitrogen. Focusing on NOR mediated by β‐Ni(OH) 2 electrode, we decipher mechanism nucleophile. For two‐step NOR, proton‐coupled electron transfer (PCET) is bridge between electrocatalytic dehydrogenation from to β‐Ni(OH)O, spontaneous dehydrogenative oxidation reaction. This theory can give good explanation for hydrazine primary amine reactions, but insufficient urea (UOR). Through operando tracing bond rupture formation processes during UOR, as well theoretical calculations, propose possible UOR whereby intramolecular coupling N−N bond, accompanied PCET, hydration rearrangement processes, results high performance ca. 100 % N selectivity. These discoveries clarify evolution molecules they elucidate fundamental aspects electrocatalysis involving nitrogen‐containing species.

Язык: Английский

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Chloride-mediated selective electrosynthesis of ethylene and propylene oxides at high current density

Science, Год журнала: 2020, Номер 368(6496), С. 1228 - 1233

Опубликована: Июнь 11, 2020

Charging into epoxides Ethylene oxide is a strained, reactive molecule produced on vast scale as plastics precursor. The current method of synthesis involves the direct reaction ethylene and oxygen at high temperature, but original protocol relied reduction chlorine to produce chlorohydrin intermediate. Leow et al. report room temperature that returns route uses electrochemistry generate it catalytically from chloride (see Perspective by Barton). This efficient process water in place can be integrated with electrochemical generation carbon dioxide. Propylene using same method. Science , this issue p. 1228 ; see also 1181

Язык: Английский

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Trimetallic Spinel NiCo_2−xFe_xO₄ Nanoboxes for Highly Efficient Electrocatalytic Oxygen Evolution

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(21), С. 11841 - 11846

Опубликована: Март 19, 2021

Abstract The development of efficient and low‐cost electrocatalysts toward the oxygen evolution reaction (OER) is critical for improving efficiency several electrochemical energy conversion storage devices. Here, we report an elaborate design synthesis porous Co‐based trimetallic spinel oxide nanoboxes (NiCo 2− x Fe O 4 NBs) by a novel metal‐organic framework engaged strategy, which involves chemical etching, cation exchange, subsequent thermal oxidation processes. Owing to structural compositional advantages, optimized NiCo NBs ( about 0.117) deliver superior electrocatalytic performance OER with overpotential 274 mV at 10 mA cm −2 , small Tafel slope 42 dec −1 good stability in alkaline electrolyte, much better than that bi/monometallic oxides even commercial RuO 2 .

Язык: Английский

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Platinum Modulates Redox Properties and 5‐Hydroxymethylfurfural Adsorption Kinetics of Ni(OH)₂ for Biomass Upgrading

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(42), С. 22908 - 22914

Опубликована: Авг. 18, 2021

Abstract Nickel hydroxide (Ni(OH) 2 ) is a promising electrocatalyst for the 5‐hydroxymethylfurfural oxidation reaction (HMFOR) and dehydronated intermediates Ni(OH)O species are proved to be active sites HMFOR. In this study, Ni(OH) modified by platinum adjust electronic structure current density of HMFOR improves 8.2 times at Pt/Ni(OH) electrode compared with that on electrode. Operando methods reveal introduction Pt optimized redox property accelerate formation during catalytic process. Theoretical studies demonstrate enhanced kinetics originates from reduced dehydrogenation energy . The product analysis transition state simulation prove also reduces adsorption HMF behavior as can act site HMF. Overall, work here provides strategy design an efficient universal nickel‐based catalyst electro‐oxidation, which extended other Ni‐based catalysts such Ni(HCO 3 NiO.

Язык: Английский

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Making electrochemistry easily accessible to the synthetic chemist

Green Chemistry, Год журнала: 2020, Номер 22(11), С. 3358 - 3375

Опубликована: Янв. 1, 2020

This tutorial bridges an important knowledge gap by providing easily accessible introduction that enables synthetic chemists to explore electrochemistry.

Язык: Английский

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Alcohols electrooxidation coupled with H2 production at high current densities promoted by a cooperative catalyst

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Янв. 10, 2022

Electrochemical alcohols oxidation offers a promising approach to produce valuable chemicals and facilitate coupled H

Язык: Английский

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