Regulating Adsorption of Intermediates via the Sulfur Modulating Dual-Atomic Sites for Boosting CO₂RR

ACS Catalysis, Год журнала: 2024, Номер 14(11), С. 8889 - 8898

Опубликована: Май 24, 2024

The formation of dual-atom catalysts or heteroatom ligand modulation is the most promising strategy for optimizing single–atom (SACs) more efficient conversion CO2 to valuable chemicals. However, ligands introduced into dual-atomic sites are expected but still under-explored. In this study, a Fe–Ni pair electrocatalyst with N– and S–coordination in porous carbon nanosheets was conceptually predicted electrocatalytic reduction CO (CO2RR). contrast SACs traditional diatomic (DACs), joined can balance cooperative activities Fe Ni sites, making adsorption configuration bidentate at both sites. This regulation leads substantial change CO* from facilitating desorption boosting CO2RR. Experimental results demonstrate that obtained FeNi–NSC catalyst achieves high selectivity Faradaic efficiencies 96.1%, remarkable activity turnover frequency 6526.9 h–1 −1.0 V, which were over 4.5 2.5 times those single work gives us insight designing highly effective guided by theoretical calculation.

Язык: Английский

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Do we achieve “1 + 1 > 2” in dual-atom or dual-single-atom catalysts?

Coordination Chemistry Reviews, Год журнала: 2024, Номер 516, С. 215961 - 215961

Опубликована: Май 29, 2024

Язык: Английский

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Recent Progress on the Stability of Electrocatalysts under High Current Densities toward Industrial Water Splitting

ACS Catalysis, Год журнала: 2024, Номер unknown, С. 14399 - 14435

Опубликована: Сен. 14, 2024

Язык: Английский

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The breakthrough of oxide pathway mechanism in stability and scaling relationship for water oxidation

National Science Review, Год журнала: 2024, Номер 11(11)

Опубликована: Окт. 15, 2024

ABSTRACT An in-depth understanding of electrocatalytic mechanisms is essential for advancing electrocatalysts the oxygen evolution reaction (OER). The emerging oxide pathway mechanism (OPM) streamlines direct O–O radical coupling, circumventing formation vacancy defects featured in lattice (LOM) and bypassing additional intermediates (*OOH) inherent to adsorbate (AEM). With only *O *OH as intermediates, OPM-driven stand out their ability disrupt traditional scaling relationships while ensuring stability. This review compiles latest significant advances OPM-based electrocatalysis, detailing design principles, synthetic methods, sophisticated techniques identify active sites pathways. We conclude with prospective challenges opportunities electrocatalysts, aiming advance field into a new era by overcoming constraints.

Язык: Английский

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Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction

Langmuir, Год журнала: 2024, Номер 40(10), С. 5469 - 5478

Опубликована: Март 4, 2024

The electrochemical nitrogen reduction reaction (eNRR) has emerged as a promising strategy for green ammonia synthesis. However, it suffers unsatisfactory performance owing to the low aqueous solubility of N2 in solution, high dissociation energy N≡N, and unavoidable competing hydrogen evolution (HER). Herein, MIL-53(Fe)@TiO2 catalyst is designed synthesized highly efficient eNRR. Relative simple MIL-53(Fe), achieves 2-fold enhancement Faradaic efficiency (FE) with an improved yield rate by 76.5% at −0.1 V versus reversible electrode (RHE). After four cycles electrocatalysis, can maintain good catalytic activity, while MIL-53(Fe) exhibits significant decrease NH3 FE 79.8 82.3%, respectively. Benefiting from synergetic effect between TiO2 composites, Fe3+ ions be greatly stabilized during eNRR process, which hinders deactivation caused ions. Further, charge transfer ability interface composites improved, thus, activity significantly boosted. These findings provide insight into preparation composite electrocatalysts.

Язык: Английский

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Single-atom vs Single-superatom as Catalysts for Ammonia Production

Chemical Communications, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

A new class of single-superatom catalyst (TiO, ZrO, and WC) supported on graphene is shown to outperform the stability activity their corresponding single-atom catalysts (Ni, Pd Pt) for electrochemical nitrogen reduction reaction. The results based density functional theory point a paradigm shift in design.

Язык: Английский

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Structural Regulation Strategies of Atomic Cobalt Catalysts for Oxygen Electrocatalysis

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 3, 2025

Abstract Oxygen electrocatalysis is a core reaction in renewable energy devices, greatly promoting the transformation and upgrading of structure. Nonetheless, performance conversion devices hindered by large overpotential slow kinetics oxygen electrocatalytic reactions. Recently, single‐atom catalysts (SACs) have emerged as promising contenders field because their exceptional metal atom utilization, distinctive coordination environment, adjustable electronic properties. This review presents latest advancements design Co‐based SACs for electrocatalysis. First, OER ORR mechanisms are introduced. Subsequently, strategies regulating structure summarized three aspects, including centers, support carriers. A particular emphasis given to relationship between properties catalysts. Afterward, applications explored. Ultimately, challenges prospects prospected.

Язык: Английский

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Advanced dual-atom catalysts for rechargeable zinc-air batteries

Energy Reviews, Год журнала: 2024, Номер 3(3), С. 100076 - 100076

Опубликована: Фев. 24, 2024

Язык: Английский

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Recent advances and future perspectives of metal-organic frameworks as efficient electrocatalysts for CO2 reduction

Science China Materials, Год журнала: 2024, Номер 68(1), С. 21 - 38

Опубликована: Ноя. 8, 2024

Abstract The conversion of carbon dioxide (CO 2 ) to the reduced chemical compounds offers substantial environmental benefits through minimizing emission greenhouse gas and fostering sustainable practices. Recently, unique properties metal-organic frameworks (MOFs) make them attractive candidates for electrocatalytic CO reduction reaction RR), providing many opportunities develop efficient, selective, environmentally processes mitigating emissions utilizing as a valuable raw material synthesis fuels chemicals. Here, recent advances in MOFs efficient catalysts RR are summarized. detailed characteristics, mechanisms, practical approaches improving efficiency, selectivity, durability under realistic conditions also clarified. Furthermore, outlooks on prospects MOF-based electrocatalysts provided.

Язык: Английский

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Selectivities of Stepped Cu–M (M = Pt, Ni, Pd, Zn, Ag, Au) Bimetallic Surface Environment for C1 and C2 Pathways

Langmuir, Год журнала: 2024, Номер 40(17), С. 9289 - 9298

Опубликована: Апрель 22, 2024

Copper (Cu) emerges as a highly efficient and cheap catalytic agent for the electrochemical reduction of carbon dioxide (CO2RR), promising sustainable route toward neutrality. Despite its utility, Cu catalyst exhibits limitations in terms product selectivity, highlighting need development superior design. Herein, we present density functional theory (DFT) investigation into selectivities Cu–M (M = Pt, Ni, Pd, Zn, Ag, Au) bimetallic catalysts (BMCs) reaction (CO2RR). The interaction between metals makes surface electrons reconstruct so that d-band center shifts to Fermi level. In CO2 activation, Cu–Ni performance. Additionally, Cu–Pd favors formation *COH along pathway, favoring generation CH4. Conversely, preferentially produces *CHO, thereby production CH3OH. For Cu–Ag catalyst, intermediates C2 pathway are *CO–*CHO *COH–*CHO. follows path proceeds via *CO–*CO → *CO–*COH *COH–CHO. On other hand, Cu–Pt sequence *OCH–*OCH. This study provides guiding significance design Cu-based aimed at improving efficiency CO2RR process.

Язык: Английский

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