Metal–Organic Framework-Based Catalysts with Single Metal Sites

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 12089 - 12174

Published: May 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.

Language: Английский

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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

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Photocatalytic CO2 reduction over metal-organic framework-based materials

Coordination Chemistry Reviews, Journal Year: 2020, Volume and Issue: 412, P. 213262 - 213262

Published: March 10, 2020

Language: Английский

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Confining isolated atoms and clusters in crystalline porous materials for catalysis

Nature Reviews Materials, Journal Year: 2020, Volume and Issue: 6(3), P. 244 - 263

Published: Oct. 23, 2020

Language: Английский

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Comprehensive Understandings into Complete Reconstruction of Precatalysts: Synthesis, Applications, and Characterizations

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(32)

Published: May 29, 2021

Reconstruction induced by external environment (such as applied voltage bias and test electrolytes) changes catalyst component catalytic behaviors. Investigations of complete reconstruction in energy conversion recently receive intensive attention, which promote the targeted design top-performance materials with maximum utilization good stability. However, advantages reconstruction, its strategies, extensive applications have not achieved profound understandings summaries it deserves. Here, this review systematically summarizes several important advances for first time, includes 1) fundamental characteristics completely reconstructed catalysts, their principles, 2) types reconstruction-involved precatalysts oxygen evolution reaction catalysis wide pH solution, origins limited degree well strategies/principles toward 3) novel material synthesis other electrocatalysis fields, 4) advanced situ/operando or multiangle/level characterization techniques to capture dynamic processes real contributors. Finally, existing major challenges unexplored/unsolved issues on studying chemistry are summarized, an outlook further development is briefly proposed. This will arouse attention diverse fields.

Language: Английский

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“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

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Advances in the Design of Heterogeneous Catalysts and Thermocatalytic Processes for CO₂ Utilization

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(23), P. 14147 - 14185

Published: Nov. 20, 2020

Utilization of CO2 as feedstock to produce fine chemicals and renewable fuels is a highly promising field, which presents unique challenges in its implementation at scale. Heterogeneous catalysis with simple operation industrial compatibility can be an effective means achieving this challenging task. This review summarizes the current developments heterogeneous thermal for production carbon monoxide, alcohols, hydrocarbons from CO2. A detailed discussion provided regarding structure–activity correlations between catalyst surface intermediate species aid rational design future generation catalysts. Effects active metal components, supports, promoters are discussed each section, will guide researchers synthesize new catalysts improved selectivity stability. Additionally, brief overview process considerations has been provided. Future research directions proposed special emphasis on application scope catalytic materials possible approaches increase performance.

Language: Английский

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MOF-enabled confinement and related effects for chemical catalyst presentation and utilization

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(3), P. 1045 - 1097

Published: Jan. 1, 2022

This review illustrates molecular-scale confinement, containment, isolation, and related concepts to present MOF-centric catalysts realize desired chemical transformations.

Language: Английский

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Homogeneous and heterogeneous catalysts for hydrogenation of CO₂ to methanol under mild conditions

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(7), P. 4259 - 4298

Published: Jan. 1, 2021

This review summarizes the concepts, mechanisms, drawbacks and challenges of state-of-the-art catalysis for CO₂ to MeOH under mild conditions. Thoughtful guidelines principles future research are presented discussed.

Language: Английский

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Highly Selective Hydrogenation of CO₂ to Ethanol via Designed Bifunctional Ir₁–In₂O₃ Single-Atom Catalyst

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(45), P. 19001 - 19005

Published: Oct. 27, 2020

Recently, CO2 hydrogenation for the controlled growth of carbon chain to produce high-value C2 or C2+ products has attracted great interest, where achieving high selectivity a specific product remains challenge, especially ethanol. Herein, we have designed bifunctional Ir1-In2O3 single-atom catalyst, integrating two active catalytic centers by anchoring monatomic Ir onto In2O3 carrier. This catalyst is efficient in liquid, yielding ethanol (>99%) with an excellent initial turnover frequency (481 h-1). Characterization shows that isolated atom couples adjacent oxygen vacancy forming Lewis acid-base pair, which activates and forms intermediate species carbonyl (CO*) adsorbed on atom. Coupling this CO* methoxide C-C bond. The strategy effective synergistically utilizing distinct roles site substrates provides new avenue design complex catalysis.

Language: Английский

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