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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Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

Nano Research, Год журнала: 2020, Номер 13(7), С. 1842 - 1855

Опубликована: Март 30, 2020

Язык: Английский

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Electronic metal–support interaction modulates single-atom platinum catalysis for hydrogen evolution reaction

Nature Communications, Год журнала: 2021, Номер 12(1)

Опубликована: Май 21, 2021

Tuning metal-support interaction has been considered as an effective approach to modulate the electronic structure and catalytic activity of supported metal catalysts. At atomic level, understanding structure-activity relationship still remains obscure in heterogeneous catalysis, such conversion water (alkaline) or hydronium ions (acid) hydrogen (hydrogen evolution reaction, HER). Here, we reveal that fine control over oxidation states single-atom Pt catalysts through significantly modulates activities either acidic alkaline HER. Combined with detailed spectroscopic electrochemical characterizations, is established by correlating acidic/alkaline HER average state Pt-H/Pt-OH interaction. This study sheds light on atomic-level mechanistic HER, further provides guidelines for rational design high-performance

Язык: Английский

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Electronic Metal–Support Interaction of Single‐Atom Catalysts and Applications in Electrocatalysis

Advanced Materials, Год журнала: 2020, Номер 32(49)

Опубликована: Окт. 30, 2020

Abstract The electronic metal–support interaction (EMSI), which acts as a bridge between theoretical study and the design of heterogenous catalysts, has attracted much attention. Utilizing metal support is one most essential strategies to enhance electrocatalytic efficiency due structural synergetic promotion. To date, ideal model for realizing EMSI, many types single‐atom catalysts (SACs) have been developed. understanding on SACs also pushed higher level. However, systematic theories operando experiments are seldom reported, will be necessary put forward carried out, respectively. Herein, types, characterization, mechanism, applications EMSI comprehensively summarized discussed. In addition basic information above, challenges, opportunities, future development proposed present an overall view reference later research.

Язык: Английский

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Intrinsic Electrocatalytic Activity Regulation of M–N–C Single‐Atom Catalysts for the Oxygen Reduction Reaction

Angewandte Chemie International Edition, Год журнала: 2020, Номер 60(9), С. 4448 - 4463

Опубликована: Апрель 21, 2020

Abstract Single‐atom catalysts (SACs) with highly active sites atomically dispersed on substrates exhibit unique advantages regarding maximum atomic efficiency, abundant chemical structures, and extraordinary catalytic performances for multiple important reactions. In particular, M–N–C SACs (M=transition metal atom) demonstrate optimal electrocatalytic activity the oxygen reduction reaction (ORR) have attracted extensive attention recently. Despite substantial efforts in fabricating various SACs, principles regulating intrinsic of their not been sufficiently studied. this Review, we summarize regulation strategies promoting ORR by modulation center atoms, coordinated environmental guest groups. Theoretical calculations experimental investigations are both included to afford a comprehensive understanding structure–performance relationship. Finally, future directions developing advanced other analogous reactions proposed.

Язык: Английский

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Coexisting Single‐Atomic Fe and Ni Sites on Hierarchically Ordered Porous Carbon as a Highly Efficient ORR Electrocatalyst

Advanced Materials, Год журнала: 2020, Номер 32(42)

Опубликована: Сен. 16, 2020

The development of oxygen reduction reaction (ORR) electrocatalysts based on earth-abundant nonprecious materials is critically important for sustainable large-scale applications fuel cells and metal-air batteries. Herein, a hetero-single-atom (h-SA) ORR electrocatalyst presented, which has atomically dispersed Fe Ni coanchored to microsized nitrogen-doped graphitic carbon support with unique trimodal-porous structure configured by highly ordered macropores interconnected through mesopores. Extended X-ray absorption fine spectra confirm that Fe- Ni-SAs are affixed the via FeN4 NiN4 coordination bonds. resultant Fe/Ni h-SA exhibits an outstanding activity, outperforming SA only or Ni-SAs, benchmark Pt/C. obtained experimental results indicate achieved performance from synergetic enhancement induced coexisting sites, superior mass-transfer capability promoted trimodal-porous-structured support.

Язык: Английский

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Recent advances of noble-metal-free bifunctional oxygen reduction and evolution electrocatalysts

Chemical Society Reviews, Год журнала: 2021, Номер 50(13), С. 7745 - 7778

Опубликована: Янв. 1, 2021

Bifunctional oxygen reduction and evolution constitute the core processes for sustainable energy storage. The advances on noble-metal-free bifunctional electrocatalysts are reviewed.

Язык: Английский

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Coordination Tunes Selectivity: Two‐Electron Oxygen Reduction on High‐Loading Molybdenum Single‐Atom Catalysts

Angewandte Chemie International Edition, Год журнала: 2020, Номер 59(23), С. 9171 - 9176

Опубликована: Март 20, 2020

Single-atom catalysts (SACs) have great potential in electrocatalysis. Their performance can be rationally optimized by tailoring the metal atoms, adjacent coordinative dopants, and loading. However, doing so is still a challenge because of limited synthesis approach insufficient understanding structure-property relationships. Herein, we report new kind Mo SAC with unique O,S coordination high loading over 10 wt %. The isolation local environment was identified high-angle annular dark-field scanning transmission electron microscopy extended X-ray absorption fine structure. SACs catalyze oxygen reduction reaction (ORR) via 2 e- pathway H2 O2 selectivity 95 % 0.10 m KOH. critical role single atoms structure revealed both electrochemical tests theoretical calculations.

Язык: Английский

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Surface/interface nanoengineering for rechargeable Zn–air batteries

Energy & Environmental Science, Год журнала: 2020, Номер 13(4), С. 1132 - 1153

Опубликована: Янв. 1, 2020

Surface/interface nanoengineering of electrocatalysts and air electrodes will promote the rapid development high-performance rechargeable Zn–air batteries.

Язык: Английский

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Coordination Engineering of Single‐Atom Catalysts for the Oxygen Reduction Reaction: A Review

Advanced Energy Materials, Год журнала: 2020, Номер 11(3)

Опубликована: Ноя. 30, 2020

Abstract Future renewable energy supplies and a sustainable environment rely on many important catalytic processes. Single‐atom catalysts (SACs) are attractive because of their maximum atom utilization efficiency, tunable electronic structures, outstanding performance. Of particular note, transition‐metal SACs exhibit excellent activity selectivity for the oxygen reduction reaction (ORR)—an half in fuel cells metal–air batteries as well portable hydrogen peroxide (H 2 O ) production. Although considerable efforts have been made synthesis ORR, regulation coordination environments thus structures still pose big challenge. In this review, strategies manipulating classified into three categories, including center metal atoms, manipulation surrounding connecting to atom, modification geometric configuration support. Finally, some issues regarding future development ORR raised possible solutions proposed.

Язык: Английский

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