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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Sabatier Relations in Electrocatalysts Based on High‐entropy Alloys with Wide‐distributed d‐band Centers for Li‐O₂ Batteries

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(44)

Опубликована: Сен. 12, 2023

Li-O2 battery (LOB) is a promising "beyond Li-ion" technology with ultrahigh theoretical energy density (3457 Wh kg-1 ), while currently impeded by the sluggish cathodic kinetics of reversible gas-solid reaction between O2 and Li2 . Despite many catalysts are developed for accelerating conversion process, lack design guidance achieving high performance makes exploring aleatory. The Sabatier principle an acknowledged theory connecting scaling relationship heterogeneous catalytic activity, providing tradeoff strategy topmost performance. Herein, series wide-distributed d-band centers (i.e., wide range adsorption strength) elaborately constructed via high-entropy strategy, enabling in-depth study relations in electrocatalysts LOBs. A volcano-type correlation center activity emerges. Both experimental results indicate that moderate appropriate strength propels up to top. As demonstration concept, LOB using FeCoNiMnPtIr as catalyst provides exceptional efficiency over 80 %, works steadily 2000 h fixed specific capacity 4000 mAh g-1 This work certifies applicability designing advanced assembled

Язык: Английский

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Emerging Strategies for the Synthesis of Correlated Single Atom Catalysts

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Фев. 9, 2024

Abstract People have been looking for an energy‐efficient and sustainable method to produce future chemicals decades. Heterogeneous single‐atom catalysts (SACs) with atomic dispersion of robust, well‐characterized active centers are highly desirable. In particular, correlated SACs cooperative interaction between adjacent single atoms allow the switching single‐site pathway dual or multisite pathway, thus promoting bimolecular more complex reactions synthesis fine chemicals. Herein, structural uniqueness SACs, including intermetal distance electronic in homo/heteronuclear metal sites is featured. Recent advances production methods showcasing research status challenges traditional (such as pyrolysis, wet impregnation, confined synthesis) building a comprehensive multimetallic SAC library, summarized. Emerging strategies such process automation continuous‐flow highlighted, minimizing inconsistency laboratory batch allowing high throughput screening upscaling toward next‐stage chemical by SACs.

Язык: Английский

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Solvent-free selective hydrogenation of nitroaromatics to azoxy compounds over Co single atoms decorated on Nb2O5 nanomeshes

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

Опубликована: Апрель 12, 2024

Abstract The solvent-free selective hydrogenation of nitroaromatics to azoxy compounds is highly important, yet challenging. Herein, we report an efficient strategy construct individually dispersed Co atoms decorated on niobium pentaoxide nanomeshes with unique geometric and electronic properties. use this supported single atom catalysts in the nitrobenzene azoxybenzene results high catalytic activity selectivity, 99% selectivity conversion within 0.5 h. Remarkably, it delivers exceptionally turnover frequency 40377 h –1 , which amongst similar state-of-the-art catalysts. In addition, demonstrates remarkable recyclability, reaction scalability, wide substrate scope. Density functional theory calculations reveal that are significantly promoted by properties strong metal-support interaction 1 /Nb 2 O 5 . absence precious metals, toxic solvents, reagents makes catalyst more appealing for synthesizing from nitroaromatics. Our findings suggest great potential access boosted thus offering blueprints design nanomaterials organocatalysis.

Язык: Английский

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A Simultaneous Modulation Strategy to Construct High Dense and Accessible Co‐N₄ Sites for Promoting Oxygen Reduction Reaction in Zn–Air Battery

Advanced Functional Materials, Год журнала: 2024, Номер 34(32)

Опубликована: Апрель 25, 2024

Abstract Transition metal‐nitrogen‐carbon single‐atom catalysts (M─N─C SACs) exhibit outstanding catalytic activity for the oxygen reduction reaction (ORR). However, these still face dual challenges of low density and utilization active sites in practical applications. Hence, a simultaneous modulation strategy to construct high‐density accessible Co‐N 4 on nitrogen‐doped porous carbon (Co H SA/NC), is reported. As expected, optimized Co SA/NC catalyst exhibits superior ORR with half‐wave potential value 0.874 V, outperforming that benchmark Pt/C catalyst. Importantly, mass turnover frequency are 14.7 13.3 times higher than low‐density single atom L respectively. Structural characterization functional theory (DFT) reveal structure high dense synergistically improve performance, which induced redistribution d orbital, resulting z 2 orbital has enough electron interact OOH * specie, thereby facilitating kinetic process ORR. Moreover, SA/NC‐based Zn–Air Battery (ZAB) also showed excellent device including high‐power (191.7 mW cm −2 ), specific capacity, stability (250 h), significantly Pt/C‐based ZABs.

Язык: Английский

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Identifying the Bifunctional Mechanism in Alkaline Water Electrolysis by Lewis Pairs at the Single-Atom Scale

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 12, 2025

The bifunctional mechanism, involving multiactive compositions to simultaneously dissociate water molecules and optimize intermediate adsorption, has been widely used in the design of catalysts boost electrolysis for sustainable hydrogen energy production but remains debatable due difficulties accurately identifying reaction process. Here, we proposed concept well-defined Lewis pairs single-atom catalysts, with a unique acid-base nature, comprehensively understand exact role an alkaline evolution reaction. By facilely adjusting active moieties, induced synergistic effect between (M-P/S/Cr pairs, M = Ru, Ir, Pt) can significantly facilitate cleavage H-OH bond accelerate removal intermediates, thereby switching rate-determining step from Volmer Heyrovsky step. Moreover, representative Ru-P deliver impressive 266 h durability at high industrial current density 2 A cm-2 without activity decay anion-exchange membrane electrolysis, be extended modify commercial noble-metal-based performance enhancement. This work not only sheds light on important mechanism scale also offers universal descriptor rational advanced catalysts.

Язык: Английский

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Breaking symmetry for better catalysis: insights into single-atom catalyst design

Chemical Society Reviews, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

This review examines the strategies of symmetry breaking (charge/coordination/geometric) in single-atom catalysts to regulate active site electronic structures, greatly enhancing catalytic performance.

Язык: Английский

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An Overview of Metal Density Effects in Single-Atom Catalysts for Thermal Catalysis

ACS Catalysis, Год журнала: 2023, Номер 13(22), С. 15126 - 15142

Опубликована: Ноя. 8, 2023

With the development of synthetic methodology, recent breakthroughs have been achieved to prepare metal single-atom catalysts (SACs) with high loadings, leading an emerging class SACs called densely populated or high-density SACs. This type provides not only higher mass-specific activity but also additional interaction among single sites, which can further influence local geometric and electronic structures individual centers thus affect intrinsic active sites. Review examines research progress atomic regulation engineering density how it affects catalytic performance in specific thermal catalysis. Last, we outline challenges prospects for future work design

Язык: Английский

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Atomic Single-Layer Ir Clusters Enabling 100% Selective Chlorine Evolution Reaction

ACS Catalysis, Год журнала: 2024, Номер 14(3), С. 1962 - 1969

Опубликована: Янв. 22, 2024

The exclusive selectivity of the chlorine evolution reaction (CER) is crucial for chlor-alkali industry to obtain pure gas and avoid cost separating byproduct oxygen. However, 100% CER remains a challenge currently known catalysts. Here, we report catalyst atomic single-layer Ir clusters on CeO2 nanorods (IrSL/CeO2). Under strong metal/support interaction, IrSL has adsorption oxygen, thereby suppressing oxygen reaction. Coupled with uniform active sites clusters, IrSL/CeO2 achieves almost in acidic NaCl solution ranging from open circuit potential practical current density levels. In addition, exhibits 1.7 times higher catalytic activity than its single-atom counterparts, noble metal efficiency 84 that commercial anodes (DSAs). Our finding provides selective catalysis electrolysis.

Язык: Английский

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Progresses and Prospects of Asymmetrically Coordinated Single Atom Catalysts for Lithium−Sulfur Batteries

Energy & environment materials, Год журнала: 2024, Номер 7(4)

Опубликована: Фев. 11, 2024

Lithium–sulfur batteries (LSBs) are widely regarded as promising next‐generation due to their high theoretical specific capacity and low material cost. However, the practical applications of LSBs limited by shuttle effect lithium polysulfides (LiPSs), electronic insulation charge discharge products, slow LiPSs conversion reaction kinetics. Accordingly, introduction catalysts into is one effective strategy solve issues sluggished LiPS conversion. Because nearly 100% atom utilization electrocatalytic activity, single‐atom (SACs) have been used mediators for LSBs' reactions. Excitingly, SACs with asymmetric coordination structures exhibited intriguing superior catalytic activities when compared traditional M–N 4 active sites. In this review, we systematically describe recent advancements in installation asymmetrically coordinated structure reactions LSBs, including nitrogen SACs, heteroatom support bimetallic SACs. Particularly noteworthy discussion mechanism spanning Finally, a perspective on future developments LSB provided.

Язык: Английский

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