Chemical Synthesis of Single Atomic Site Catalysts

Chemical Reviews, Год журнала: 2020, Номер 120(21), С. 11900 - 11955

Опубликована: Апрель 3, 2020

Manipulating metal atoms in a controllable way for the synthesis of materials with desired structure and properties is holy grail chemical synthesis. The recent emergence single atomic site catalysts (SASC) demonstrates that we are moving toward this goal. Owing to maximum efficiency atom-utilization unique structures properties, SASC have attracted extensive research attention interest. prerequisite scientific practical applications fabricate highly reactive stable on appropriate supports. In review, various synthetic strategies summarized concrete examples highlighting key issues methods stabilize supports suppress their migration agglomeration. Next, discuss how conditions affect catalytic before ending review by prospects challenges as well further researches SASC.

Язык: Английский

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Industrial carbon dioxide capture and utilization: state of the art and future challenges

Chemical Society Reviews, Год журнала: 2020, Номер 49(23), С. 8584 - 8686

Опубликована: Янв. 1, 2020

This review covers the sustainable development of advanced improvements in CO₂capture and utilization.

Язык: Английский

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Metal–Organic Framework-Based Catalysts with Single Metal Sites

Chemical Reviews, Год журнала: 2020, Номер 120(21), С. 12089 - 12174

Опубликована: Май 1, 2020

Metal-organic frameworks (MOFs) are a class of distinctive porous crystalline materials constructed by metal ions/clusters and organic linkers. Owing to their structural diversity, functional adjustability, high surface area, different types MOF-based single sites well exploited, including coordinately unsaturated from nodes metallolinkers, as active species immobilized MOFs. Furthermore, controllable thermal transformation MOFs can upgrade them nanomaterials functionalized with single-atom catalysts (SACs). These unique features derivatives enable serve highly versatile platform for catalysis, which has actually been becoming rapidly developing interdisciplinary research area. In this review, we overview the recent developments catalysis at in emphasis on structures applications thermocatalysis, electrocatalysis, photocatalysis. We also compare results summarize major insights gained works providing challenges prospects emerging field.

Язык: Английский

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Electrocatalysis for CO₂conversion: from fundamentals to value-added products

Chemical Society Reviews, Год журнала: 2021, Номер 50(8), С. 4993 - 5061

Опубликована: Янв. 1, 2021

This timely and comprehensive review mainly summarizes advances in heterogeneous electroreduction of CO₂: from fundamentals to value-added products.

Язык: Английский

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Tuning the Coordination Environment in Single-Atom Catalysts to Achieve Highly Efficient Oxygen Reduction Reactions

Journal of the American Chemical Society, Год журнала: 2019, Номер 141(51), С. 20118 - 20126

Опубликована: Дек. 5, 2019

Designing atomically dispersed metal catalysts for oxygen reduction reaction (ORR) is a promising approach to achieve efficient energy conversion. Herein, we develop template-assisted method synthesize series of single atoms anchored on porous N,S-codoped carbon (NSC) matrix as highly ORR investigate the correlation between structure and their catalytic performance. The analysis indicates that an identical synthesis results in distinguished structural differences Fe-centered single-atom catalyst (Fe-SAs/NSC) Co-centered/Ni-centered (Co-SAs/NSC Ni-SAs/NSC) because different trends each ion forming complex with N,S-containing precursor during initial process. Fe-SAs/NSC mainly consists well-dispersed FeN4S2 center site where S form bonds N atoms. Co-SAs/NSC Ni-SAs/NSC, other hand, metal–S bonds, resulting CoN3S1 NiN3S1 sites. Density functional theory (DFT) reveals more active than sites, due higher charge density, lower barriers intermediates, products involved. experimental indicate all three could contribute high electrochemical performances, while exhibits highest all, which even better commercial Pt/C. Furthermore, also displays methanol tolerance compared Pt/C stability up 5000 cycles. This work provides insights into rational design definitive tunable electrocatalytic activities

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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Surface strategies for catalytic CO₂reduction: from two-dimensional materials to nanoclusters to single atoms

Chemical Society Reviews, Год журнала: 2019, Номер 48(21), С. 5310 - 5349

Опубликована: Янв. 1, 2019

This work constructively reviewed and predicted the surface strategies for catalytic CO₂reduction with 2D material, nanocluster single-atom catalysts

Язык: Английский

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Atomic site electrocatalysts for water splitting, oxygen reduction and selective oxidation

Chemical Society Reviews, Год журнала: 2020, Номер 49(7), С. 2215 - 2264

Опубликована: Янв. 1, 2020

This review summarized the fabrication routes and characterization methods of atomic site electrocatalysts (ASCs) followed by their applications for water splitting, oxygen reduction selective oxidation.

Язык: Английский

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Bismuth Single Atoms Resulting from Transformation of Metal–Organic Frameworks and Their Use as Electrocatalysts for CO₂ Reduction

Journal of the American Chemical Society, Год журнала: 2019, Номер 141(42), С. 16569 - 16573

Опубликована: Окт. 5, 2019

The electrocatalytic reduction reaction of CO2 (CO2RR) is a promising strategy to promote the global carbon balance and combat climate change. Herein, exclusive Bi-N4 sites on porous networks can be achieved through thermal decomposition bismuth-based metal-organic framework (Bi-MOF) dicyandiamide (DCD) for CO2RR. Interestingly, in situ environmental transmission electron microscopy (ETEM) analysis not only directly shows from Bi-MOF into Bi nanoparticles (NPs) but also exhibits subsequent atomization NPs assisted by NH3 released DCD. Our catalyst high intrinsic activity CO conversion, with Faradaic efficiency (FECO up 97%) turnover frequency 5535 h-1 at low overpotential 0.39 V versus reversible hydrogen electrode. Further experiments density functional theory results demonstrate that single-atom site dominating active center simultaneously activation rapid formation key intermediate COOH* free energy barrier.

Язык: Английский

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Molecular enhancement of heterogeneous CO2 reduction

Nature Materials, Год журнала: 2020, Номер 19(3), С. 266 - 276

Опубликована: Фев. 25, 2020

Язык: Английский

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