Non-noble metal-nitride based electrocatalysts for high-performance alkaline seawater electrolysis

Nature Communications, Год журнала: 2019, Номер 10(1)

Опубликована: Ноя. 8, 2019

Abstract Seawater is one of the most abundant natural resources on our planet. Electrolysis seawater not only a promising approach to produce clean hydrogen energy, but also great significance desalination. The implementation electrolysis requires robust and efficient electrocatalysts that can sustain splitting without chloride corrosion, especially for anode. Here we report three-dimensional core-shell metal-nitride catalyst consisting NiFeN nanoparticles uniformly decorated NiMoN nanorods supported Ni foam, which serves as an eminently active durable oxygen evolution reaction alkaline electrolysis. Combined with nanorods, have achieved industrially required current densities 500 1000 mA cm −2 at record low voltages 1.608 1.709 V, respectively, overall 60 °C. This discovery significantly advances development large-scale production.

Язык: Английский

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Single-Atom Catalysts across the Periodic Table

Chemical Reviews, Год журнала: 2020, Номер 120(21), С. 11703 - 11809

Опубликована: Окт. 21, 2020

Isolated atoms featuring unique reactivity are at the heart of enzymatic and homogeneous catalysts. In contrast, although concept has long existed, single-atom heterogeneous catalysts (SACs) have only recently gained prominence. Host materials similar functions to ligands in catalysts, determining stability, local environment, electronic properties isolated thus providing a platform for tailoring targeted applications. Within just decade, we witnessed many examples SACs both disrupting diverse fields catalysis with their distinctive substantially enriching our understanding molecular processes on surfaces. To date, term SAC mostly refers late transition metal-based systems, but numerous exist which other elements play key catalytic roles. This review provides compositional encyclopedia SACs, celebrating 10th anniversary introduction this term. By defining broadest sense, explore full elemental diversity, joining different areas across whole periodic table, discussing historical milestones recent developments. particular, examine coordination structures associated accessed through distinct single-atom–host combinations relate them main applications thermo-, electro-, photocatalysis, revealing trends element-specific evolution, host design, uses. Finally, highlight frontiers field, including multimetallic atom proximity control, possible multistep cascade reactions, identifying challenges, propose directions future development flourishing field.

Язык: Английский

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Advanced Electrocatalysts with Single-Metal-Atom Active Sites

Chemical Reviews, Год журнала: 2020, Номер 120(21), С. 12217 - 12314

Опубликована: Ноя. 2, 2020

Electrocatalysts with single metal atoms as active sites have received increasing attention owing to their high atomic utilization efficiency and exotic catalytic activity selectivity. This review aims provide a comprehensive summary on the recent development of such single-atom electrocatalysts (SAECs) for various energy-conversion reactions. The discussion starts an introduction different types SAECs, followed by overview synthetic methodologies control dispersion atomically resolved characterization using state-of-the-art microscopic spectroscopic techniques. In recognition extensive applications electrocatalytic studies are dissected in terms important electrochemical reactions, including hydrogen evolution reaction (HER), oxygen (OER), reduction (ORR), carbon dioxide (CO2RR), nitrogen (NRR). Examples SAECs deliberated each case performance, structure-property relationships, enhancement mechanisms. A perspective is provided at end section about remaining challenges opportunities targeted reaction.

Язык: Английский

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Recent Advances in Design of Electrocatalysts for High‐Current‐Density Water Splitting

Advanced Materials, Год журнала: 2021, Номер 34(16)

Опубликована: Дек. 4, 2021

Abstract Electrochemical water splitting technology for producing “green hydrogen” is important the global mission of carbon neutrality. Electrocatalysts with decent performance at high current densities play a central role in industrial implementation this technology. This field has advanced immensely recent years, as witnessed by many types catalysts designed and synthesized toward industriallyrelevant (>200 mA cm –2 ). By discussing advances field, several key aspects are summarized that affect catalytic high‐current‐density electrocatalysis, including dimensionality catalysts, surface chemistry, electron transport path, morphology, catalyst‐electrolyte interplay. The multiscale design strategy considers these comprehensively developing electrocatalysts highlighted. perspectives on future directions emerging also put forward.

Язык: Английский

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Structural Transformation of Heterogeneous Materials for Electrocatalytic Oxygen Evolution Reaction

Chemical Reviews, Год журнала: 2021, Номер 121(21), С. 13174 - 13212

Опубликована: Сен. 15, 2021

Electrochemical water splitting for hydrogen generation is a promising pathway renewable energy conversion and storage. One of the most important issues efficient to develop cost-effective highly electrocatalysts drive sluggish oxygen-evolution reaction (OER) at anode side. Notably, structural transformation such as surface oxidation metals or metal nonoxide compounds amorphization some oxides during OER have attracted growing attention in recent years. The investigation will contribute in-depth understanding accurate catalytic mechanisms finally benefit rational design materials with high activity. In this Review, we provide an overview heterogeneous obvious electrocatalysis. To gain insight into essence transformation, summarize driving forces critical factors that affect process. addition, advanced techniques are used probe chemical states atomic structures transformed surfaces also introduced. We then discuss structure active species relationship between performance properties materials. Finally, challenges prospects electrocatalysis presented.

Язык: Английский

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Synergistic Modulation of Non-Precious-Metal Electrocatalysts for Advanced Water Splitting

Accounts of Chemical Research, Год журнала: 2020, Номер 53(6), С. 1111 - 1123

Опубликована: Май 28, 2020

ConspectusHydrogen is an ideal energy carrier and plays a critical role in the future transition. Distinct from steam reforming, electrochemical water splitting, especially powered by renewables, has been considered as promising technique for scalable production of high-purity hydrogen with no carbon emission. Its commercialization relies on reduction electricity consumption thus cost, calling highly efficient cost-effective electrocatalysts capability steadily working at high output. This requires to feature (1) active intrinsic sites, (2) abundant accessible (3) effective electron mass transfer, (4) chemical structural durability, (5) low-cost synthesis. It should be noted that all these requirements fulfilled together practicable electrocatalyst. Much effort devoted addressing one or few aspects, improving electrocatalytic activity electronic modulation while reviews have focused synergistic aspects although it essential advanced splitting.In this Account, we will present recent innovative strategies emphasis our solutions synergistically modulating transportation, gas evolution, well mechanical non-precious-metal electrocatalysts, aiming splitting. The following approaches coupling are summarized both cathodic evolution reaction (HER) anodic oxygen (OER). Synergistic modulations. structure catalytic site determines adsorption/desorption reactive intermediates activity. can tuned heterogeneous doping, strain effect, spin polarization, etc. Coupling effects optimize pathways target simultaneously stability would advance performance. crystalline modulation. crystallinity, phase, facets, defects, affect stability. enhance morphological focus concurrently morphology increasing through single action processing. transfer properties also enhanced enable splitting large elementary reactions. Electrocatalytic generally consists couple Each may need specific site. Designing combining various components targeting every step space-limited catalyst surface balance steps accelerating overall reaction. Integrated electrocatalyst design. Taking into account necessary integrate above features enabling high-output electrolysis. Beyond progress made date, remaining challenges opportunities discussed. With insights, hopefully, Account shed light rational design practical water-splitting hydrogen.

Язык: Английский

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Unveiling the Promotion of Surface‐Adsorbed Chalcogenate on the Electrocatalytic Oxygen Evolution Reaction

Angewandte Chemie International Edition, Год журнала: 2020, Номер 59(50), С. 22470 - 22474

Опубликована: Сен. 10, 2020

Transition metal chalcogenides (TMCs) are efficient oxygen evolution reaction (OER) pre-electrocatalysts, and will in situ transform into (oxy)hydroxides under OER condition. However, the role of chalcogen is not fully elucidated after oxidation severe leaching. Here we present vital promotion surface-adsorbed chalcogenates on activity. Taking NiSe2 as an example, Raman spectroscopy revealed Se-Se to selenites (SeO32- ) then selenates (SeO42- ). Combining Se leaching strong signal selenates, it assumed that rich surface play significant roles. As expected, adding electrolyte Ni(OH)2 dramatically enhance its And sulfates also exhibit similar effect, suggesting universal. Our findings offer unique insight transformation mechanism materials during electrolysis.

Язык: Английский

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Understanding of Oxygen Redox in the Oxygen Evolution Reaction

Advanced Materials, Год журнала: 2022, Номер 34(50)

Опубликована: Июль 20, 2022

The electron-transfer process during the oxygen evolution reaction (OER) often either proceeds solely via a metal redox chemistry (adsorbate mechanism (AEM), with bands around Fermi level) or an (lattice oxidation (LOM), level). Unlike AEM, LOM involves instead of redox, which leads to formation direct oxygen-oxygen (OO) bond. As result, such is able bypass rate-determining step, that is, OO bonding, in highlights critical advantage as compared conventional AEM. Thus, it has been well reported LOM-based catalysts are demonstrate higher OER activities AEM-based catalysts. Here, comprehensive understanding and all documented possible characterization techniques can be used identify reviewed. This review will interpret origins electrocatalysts underlying science LOM-induced surface reconstruction transition oxides. Finally, perspectives on future development also provided.

Язык: Английский

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An Engineered Superhydrophilic/Superaerophobic Electrocatalyst Composed of the Supported CoMoS_x Chalcogel for Overall Water Splitting

Angewandte Chemie International Edition, Год журнала: 2019, Номер 59(4), С. 1659 - 1665

Опубликована: Окт. 23, 2019

The development of high-efficiency electrocatalysts for large-scale water splitting is critical but also challenging. In this study, a hierarchical CoMoSx chalcogel was synthesized on nickel foam (NF) through an in situ metathesis reaction and demonstrated excellent activity stability the electrocatalytic hydrogen evolution oxygen alkaline media. high catalytic could be ascribed to abundant active sites/defects amorphous framework promotion cobalt doping. Furthermore, superhydrophilicity superaerophobicity micro-/nanostructured /NF promoted mass transfer by facilitating access electrolytes ensuring fast release gas bubbles. By employing as bifunctional electrocatalysts, overall device delivered current density 500 mA cm-2 at low voltage 1.89 V maintained its without decay 100 h.

Язык: Английский

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Oxygen Evolution/Reduction Reaction Catalysts: From In Situ Monitoring and Reaction Mechanisms to Rational Design

Chemical Reviews, Год журнала: 2023, Номер 123(9), С. 6257 - 6358

Опубликована: Март 21, 2023

The oxygen evolution reaction (OER) and reduction (ORR) are core steps of various energy conversion storage systems. However, their sluggish kinetics, i.e., the demanding multielectron transfer processes, still render OER/ORR catalysts less efficient for practical applications. Moreover, complexity catalyst–electrolyte interface makes a comprehensive understanding intrinsic mechanisms challenging. Fortunately, recent advances in situ/operando characterization techniques have facilitated kinetic monitoring under conditions. Here we provide selected highlights mechanistic studies with main emphasis placed on heterogeneous systems (primarily discussing first-row transition metals which operate basic conditions), followed by brief outlook molecular catalysts. Key sections this review focused determination true active species, identification sites, reactive intermediates. For in-depth insights into above factors, short overview metrics accurate characterizations is provided. A combination obtained time-resolved information reliable activity data will then guide rational design new Strategies such as optimizing restructuring process well overcoming adsorption-energy scaling relations be discussed. Finally, pending current challenges prospects toward development homogeneous presented.

Язык: Английский

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