High Entropy Alloy Electrocatalytic Electrode toward Alkaline Glycerol Valorization Coupling with Acidic Hydrogen Production

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(16), С. 7224 - 7235

Опубликована: Апрель 11, 2022

Electrochemical glycerol oxidation reaction (GOR) is an attractive alternative anodic to oxygen evolution for a variety of electrolytic synthesis, thanks the possibility mass production from biomass and relative low thermodynamic potential GOR. The development high-activity cheap electrocatalysts toward GOR yet faces daunting challenge. Herein, we experimentally prepare new range high entropy alloy (HEA) self-supported electrodes with uniform HEA nanoparticles grown on carbon cloth. systematic electrochemical studies verify that HEA-CoNiCuMnMo electrode exhibits performance electrocatalysis overpotential selectivity formate products. surface atomic configurations are studied by self-developed machine learning-based Monte Carlo simulation, which points out catalytic active center be Mo sites coordinated Mn, Mo, Ni. We further develop hybrid alkali/acid flow cell pairing alkaline acidic hydrogen using commercial RhIr/Ti as anode cathode, respectively, only requires applied voltage 0.55 V reach current density 10 mA cm-2 maintains long-term electrolysis stability over 12 days continuous running at 50 Faraday efficiencies 99% H2 in cathode 92% anode.

Язык: Английский

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Status and perspectives of key materials for PEM electrolyzer

Deleted Journal, Год журнала: 2022, Номер 1, С. e9120032 - e9120032

Опубликована: Сен. 8, 2022

Proton exchange membrane water electrolyzer (PEMWE) represents a promising technology for the sustainable production of hydrogen, which is capable efficiently coupling to intermittent electricity from renewable energy sources (e.g., solar and wind). The with compact stack structure has many notable advantages, including large current density, high hydrogen purity, great conversion efficiency. However, use expensive electrocatalysts construction materials leads costs limited application. In this review, recent advances made in key PEMWE are summarized. First, we present brief overview about basic principles, thermodynamics, reaction kinetics PEMWE. We then describe cell components their respective functions, as well discuss research status such membrane, electrocatalysts, electrode assemblies, gas diffusion layer, bipolar plate. also attempt clarify degradation mechanisms under real operating environment, catalyst degradation, plate layer degradation. finally propose several future directions developing through devoting more efforts materials.

Язык: Английский

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A high-entropy atomic environment converts inactive to active sites for electrocatalysis

Energy & Environmental Science, Год журнала: 2023, Номер 16(2), С. 619 - 628

Опубликована: Янв. 1, 2023

An electronegativity-dominant high-entropy atomic environment regulation strategy was developed to manipulate the electrocatalytic properties by tailoring competitive adsorption sites in HEA NPs.

Язык: Английский

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Hydrogen production by water electrolysis technologies: A review

Results in Engineering, Год журнала: 2023, Номер 20, С. 101426 - 101426

Опубликована: Сен. 19, 2023

Hydrogen as an energy source has been identified optimal pathway for mitigating climate change by combining renewable electricity with water electrolysis systems. Proton exchange membrane (PEM) technology received a substantial amount of attention because its ability to efficiently produce high-purity hydrogen while minimising challenges associated handling and maintenance. Another generation technology, alkaline (AWE), widely used in commercial production applications. Anion (AEM) can at relatively low costs the noble metal catalysts PEM AWE systems are replaced conventional low-cost electrocatalysts. Solid oxide electrolyzer cell (SOEC) is another producing high conversion efficiencies, cost, emissions. However, operating temperatures SOECs which necessitates long startup times. This review addresses current state technologies capable using impure Commercially available were extensively discussed compared. The technical barriers AEM also investigated. Furthermore, stack performance was evaluated artificial river (soft water). An integrated system approach recommended meeting power pure demands reversible seawater electricity, electrolysis, fuel cells. considered be low, requiring further developments enhance membrane's lifetime.

Язык: Английский

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Manipulating the Water Dissociation Electrocatalytic Sites of Bimetallic Nickel‐Based Alloys for Highly Efficient Alkaline Hydrogen Evolution

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(30)

Опубликована: Апрель 20, 2022

Transition-metal alloys are currently drawing increasing attention as promising electrocatalysts for the alkaline hydrogen evolution reaction (HER). However, traditional density-functional-theory-derived d-band theory fails to describe adsorption energy (ΔGH ) on hollow sites. Herein, by studying ΔGH a series of Ni-M (M=Ti, V, Cr, Mn, Fe, Co, Cu, Zn, Mo, W) bimetallic alloys, an improved center was provided and potential NiCu electrocatalyst with near-optimal discovered. Moreover, oxygen atoms were introduced into (O-NiM) balance adsorption/desorption hydroxyl species. The tailored electrocatalytic sites water dissociation can synergistically accelerate multi-step HER. prepared O-NiCu shows optimum HER activity low overpotential 23 mV at 10 mA cm-2 . This work not only broadens applicability theory, but also provides crucial understanding designing efficient electrocatalysts.

Язык: Английский

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

Carbon Neutrality, Год журнала: 2022, Номер 1(1)

Опубликована: Июнь 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.

Язык: Английский

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Work‐function‐induced Interfacial Built‐in Electric Fields in Os‐OsSe₂Heterostructures for Active Acidic and Alkaline Hydrogen Evolution

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(36)

Опубликована: Июль 13, 2022

Theoretical calculations unveil that the formation of Os-OsSe2 heterostructures with neutralized work function (WF) perfectly balances electronic state between strong (Os) and weak (OsSe2 ) adsorbents bidirectionally optimizes hydrogen evolution reaction (HER) activity Os sites, significantly reducing thermodynamic energy barrier accelerating kinetics process. Then, heterostructural is constructed for first time by a molten salt method confirmed in-depth structural characterization. Impressively, due to highly active sites endowed charge balance effect, exhibits ultra-low overpotentials HER in both acidic (26 mV @ 10 mA cm-2 alkaline (23 media, surpassing commercial Pt catalysts. Moreover, solar-to-hydrogen device assembled further highlights its potential application prospects. Profoundly, this special heterostructure provides new model rational selection heterocomponents.

Язык: Английский

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Noble-Metal High-Entropy-Alloy Nanoparticles: Atomic-Level Insight into the Electronic Structure

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(8), С. 3365 - 3369

Опубликована: Фев. 15, 2022

The compositional space of high-entropy-alloy nanoparticles (HEA NPs) significantly expands the diversity materials library. Every atom in HEA NPs has a different elemental coordination environment, which requires knowledge local electronic structure at an atomic level. However, such not been disclosed experimentally or theoretically. We synthesized composed all eight noble-metal-group elements (NM-HEA) for first time. Their was revealed by hard X-ray photoelectron spectroscopy and density function theory calculations with NP models. NM-HEA have lower degeneracy energy level compared monometallic NPs, is common feature NPs. states (LDOS) every surface revealed. Some atoms same constituent element LDOS profiles, whereas other similar profiles. In words, one loses its identity it may be possible to create ideal adjusting neighboring atoms. tendency change shown supervised learning. showed 10.8-times higher intrinsic activity hydrogen evolution reaction than commercial Pt/C, best catalysts.

Язык: Английский

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Recent progress on the long‐term stability of hydrogen evolution reaction electrocatalysts

InfoMat, Год журнала: 2022, Номер 4(9)

Опубликована: Авг. 23, 2022

Abstract Developing new methodologies to produce clean and renewable energy resources is pivotal for carbon‐neutral initiatives. Hydrogen (H 2 ) considered as an ideal resource due its nontoxic, pollution‐free, high utilization rate, calorific combustion value. Electrolysis of water driven by the electricity generated from sources (e.g., solar energy, wind energy) hydrogen attracts great efforts production with purity. Recently, breakthrough catalyst activity limit evolution reaction (HER) catalysts has received extensive attention. Comparatively, fewer reviews have focused on long‐term stability HER catalysts, which indeed decisive large‐scale electrolytic industrialization. Therefore, a systematic summary concentrated durability electrocatalysts would provide fundamental understanding electrocatalytic performance practical applications offer opportunities rational design highly performed electrocatalysts. This review summarizes research progress toward precious metals, transition metal‐free in past few years. It discusses challenges future perspectives. We anticipate that it valuable basis designing robust image

Язык: Английский

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High‐Entropy Intermetallic PtRhBiSnSb Nanoplates for Highly Efficient Alcohol Oxidation Electrocatalysis

Advanced Materials, Год журнала: 2022, Номер 34(43)

Опубликована: Сен. 5, 2022

The control of multimetallic ensembles at the atomic-level is challenging, especially for high-entropy alloys (HEAs) possessing five or more elements. Herein, one-pot synthesis hexagonal-close-packed (hcp) PtRhBiSnSb intermetallic (HEI) nanoplates with intrinsically isolated Pt, Rh, Bi, Sn, and Sb atoms reported, to boost electrochemical oxidation liquid fuels. Taking advantage these combined metals, well-defined HEI exhibit a remarkable mass activity 19.529, 15.558, 7.535 A mg-1Pt+Rh toward electrooxidation methanol, ethanol, glycerol in alkaline electrolytes, respectively, representing state-of-the-art multifunctional electrocatalyst alcohol reactions. In particular, achieves record-high methanol reaction (MOR) an environment. Theoretical calculations demonstrate that introduction fifth metal Rh enhances electron-transfer efficiency nanoplates, which contributes improved capability. Meanwhile, robust electronic structures active sites are achieved due synergistic protections from sites. This work offers significant research advances developing HEA delicate over compositions properties.

Язык: Английский

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