Single-Atom Catalysts across the Periodic Table

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 11703 - 11809

Published: Oct. 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.

Language: Английский

---

Tackling the Activity and Selectivity Challenges of Electrocatalysts toward the Nitrogen Reduction Reaction via Atomically Dispersed Biatom Catalysts

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(12), P. 5709 - 5721

Published: Feb. 18, 2020

Developing efficient catalysts for nitrogen fixation is becoming increasingly important but still challenging due to the lack of robust design criteria tackling activity and selectivity problems, especially electrochemical reduction reaction (NRR). Herein, by means large-scale density functional theory (DFT) computations, we reported a descriptor-based principle explore large composition space two-dimensional (2D) biatom (BACs), namely, metal dimers supported on 2D expanded phthalocyanine (M2-Pc or MM'-Pc), toward NRR at acid conditions. We sampled both homonuclear (M2-Pc) heteronuclear (MM'-Pc) BACs constructed map using N2H* adsorption energy as descriptor, which reduces number promising catalyst candidates from over 900 less than 100. This strategy allowed us readily identify 3 28 BACs, could break metal-based benchmark NRR. Particularly, free difference H* screened out five systems, including Ti2-Pc, V2-Pc, TiV-Pc, VCr-Pc, VTa-Pc, exhibit strong capability suppressing competitive hydrogen evolution (HER) with favorable limiting potential -0.75, -0.39, -0.74, -0.85, -0.47 V, respectively. work not only broadens possibility discovering more N2 also provides feasible rational electrocatalysts helps pave way fast screening other reactions.

Language: Английский

---

Emerging Dual‐Atomic‐Site Catalysts for Efficient Energy Catalysis

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(36)

Published: July 23, 2021

Atomically dispersed metal catalysts with well-defined structures have been the research hotspot in heterogeneous catalysis because of their high atomic utilization efficiency, outstanding activity, and selectivity. Dual-atomic-site (DASCs), as an extension single-atom (SACs), recently drawn surging attention. The DASCs possess higher loading, more sophisticated flexible active sites, offering chance for achieving better catalytic performance, compared SACs. In this review, recent advances on how to design new enhancing energy will be highlighted. It start classification marriage two kinds homonuclear heteronuclear according configuration sites. Then, state-of-the-art characterization techniques discussed. Different synthetic methods applications various reactions, including oxygen reduction reaction, carbon dioxide monoxide oxidation others followed. Finally, major challenges perspectives provided.

Language: Английский

---

Noble-metal single-atoms in thermocatalysis, electrocatalysis, and photocatalysis

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(5), P. 2954 - 3009

Published: Jan. 1, 2021

This review summarizes the recent advances about noble-metal single-atom catalysts in thermocatalysis, electrocatalysis, and photocatalysis.

Language: Английский

---

Structural Regulation with Atomic-Level Precision: From Single-Atomic Site to Diatomic and Atomic Interface Catalysis

Matter, Journal Year: 2020, Volume and Issue: 2(1), P. 78 - 110

Published: Jan. 1, 2020

Language: Английский

---

“More is Different:” Synergistic Effect and Structural Engineering in Double‐Atom Catalysts

Advanced Functional Materials, Journal Year: 2020, Volume and Issue: 31(3)

Published: Nov. 16, 2020

Abstract Double‐atom catalysts (DACs) have emerged as a novel frontier in heterogeneous catalysis because the synergistic effect between adjacent active sites can promote their catalytic activity while maintaining high atomic utilization efficiency, good selectivity, and stability originating from atomically dispersed nature. In this review, recent progress both experimental theoretical research on DACs for various reactions is focused. Specifically, central tasks design of DACs—manipulating engineering electronic structures catalysts—are systematically reviewed, along with prevailing experimental, characterization, computational modeling approaches. Furthermore, practical applications water splitting, oxygen reduction reaction, nitrogen carbon dioxide reaction are addressed. Finally, future challenges summarized an outlook further investigations toward high‐performance energy environmental provided.

Language: Английский

---

Bimetallic Sites for Catalysis: From Binuclear Metal Sites to Bimetallic Nanoclusters and Nanoparticles

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(8), P. 4855 - 4933

Published: March 27, 2023

Heterogeneous bimetallic catalysts have broad applications in industrial processes, but achieving a fundamental understanding on the nature of active sites at atomic and molecular level is very challenging due to structural complexity catalysts. Comparing features catalytic performances different entities will favor formation unified structure-reactivity relationships heterogeneous thereby facilitate upgrading current In this review, we discuss geometric electronic structures three representative types (bimetallic binuclear sites, nanoclusters, nanoparticles) then summarize synthesis methodologies characterization techniques for entities, with emphasis recent progress made past decade. The supported nanoparticles series important reactions are discussed. Finally, future research directions catalysis based and, more generally, prospective developments both practical applications.

Language: Английский

---

Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis

Nano Research, Journal Year: 2022, Volume and Issue: 15(9), P. 7806 - 7839

Published: June 2, 2022

Language: Английский

---

Metal-metal interactions in correlated single-atom catalysts

Science Advances, Journal Year: 2022, Volume and Issue: 8(17)

Published: April 29, 2022

Single-atom catalysts (SACs) include a promising family of electrocatalysts with unique geometric structures. Beyond conventional ones fully isolated metal sites, an emerging class the adjacent single atoms exhibiting intersite metal-metal interactions appear in recent years and can be denoted as correlated SACs (C-SACs). This type provides more opportunities to achieve substantial structural modification performance enhancement toward wider range electrocatalytic applications. On basis clear identification interactions, this review critically examines research progress C-SACs. It shows that control enables regulation atomic structure, local coordination, electronic properties atoms, which facilitate modulation behavior Last, we outline directions for future work design development C-SACs, is indispensable creating high-performing new SAC architectures.

Language: Английский

---

Surface Reorganization on Electrochemically‐Induced Zn–Ni–Co Spinel Oxides for Enhanced Oxygen Electrocatalysis

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 59(16), P. 6492 - 6499

Published: Jan. 27, 2020

Herein, we highlight redox-inert Zn2+ in spinel-type oxide (ZnX Ni1-X Co2 O4 ) to synergistically optimize physical pore structure and increase the formation of active species on catalyst surface. The presence segregation has been identified experimentally theoretically under oxygen-evolving condition, newly formed VZn -O-Co allows more suitable binding interaction between center Co oxygenated species, resulting superior ORR performance. Moreover, a liquid flow Zn-air battery is constituted employing structurally optimized Zn0.4 Ni0.6 nanoparticles supported N-doped carbon nanotube (ZNCO/NCNTs) as an efficient air cathode, which presents remarkable power density (109.1 mW cm-2 ), high open circuit potential (1.48 V vs. Zn), excellent durability, high-rate This finding could elucidate observed enhancement activity ZnX oxides after OER test.

Language: Английский

---