State of the Art and Prospects in Metal–Organic Framework (MOF)-Based and MOF-Derived Nanocatalysis

Chemical Reviews, Journal Year: 2019, Volume and Issue: 120(2), P. 1438 - 1511

Published: June 27, 2019

Metal–organic framework (MOF) nanoparticles, also called porous coordination polymers, are a major part of nanomaterials science, and their role in catalysis is becoming central. The extraordinary variability richness structures afford engineering synergies between the metal nodes, functional linkers, encapsulated substrates, or nanoparticles for multiple selective heterogeneous interactions activations these MOF-based nanocatalysts. Pyrolysis MOF-nanoparticle composites forms highly N- P-doped graphitized MOF-derived that increasingly used as efficient catalysts especially electro- photocatalysis. This review first briefly summarizes this background MOF nanoparticle then comprehensively reviews fast-growing literature reported during last years. parts organic molecular reactions, electrocatalysis, photocatalysis, views prospects. Major challenges our society addressed using well-defined fields synthesis, energy, environment. In spite many achievements, enormous progress still necessary to improve understanding processes involved beyond proof-of-concept, particularly methane oxidation, hydrogen production, water splitting, CO2 reduction methanol, nitrogen fixation, depollution.

Language: Английский

---

Chemical Synthesis of Single Atomic Site Catalysts

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 11900 - 11955

Published: April 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.

Language: Английский

---

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

---

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

---

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

---

Heterogeneous Single-Atom Photocatalysts: Fundamentals and Applications

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 12175 - 12216

Published: March 18, 2020

Single-atom photocatalysts have shown their compelling potential and arguably become the most active research direction in photocatalysis due to fascinating strengths enhancing light-harvesting, charge transfer dynamics, surface reactions of a photocatalytic system. While numerous comprehensions about single-atom recently been amassed, advanced characterization techniques vital theoretical studies are strengthening our understanding on these materials, allowing us forecast working mechanisms applications photocatalysis. In this review, we begin by describing general background definition photocatalysts. A brief discussion metal-support interactions is then provided. Thereafter, current available for summarized. After having some fundamental photocatalysts, advantages discussed. Finally, end review with look into remaining challenges future perspectives We anticipate that will provide inspiration discovery manifestly stimulating development emerging area.

Language: Английский

---

Artificial photosynthesis: opportunities and challenges of molecular catalysts

Chemical Society Reviews, Journal Year: 2019, Volume and Issue: 48(7), P. 2216 - 2264

Published: Jan. 1, 2019

This review emphasizes the significance of molecular catalysts in artificial photosynthesis, and discusses opportunities, challenges future catalysis.

Language: Английский

---

Single-atom catalysis in advanced oxidation processes for environmental remediation

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(8), P. 5281 - 5322

Published: Jan. 1, 2021

This review presents the recent advances in synthetic strategies, characterisation, and computations of carbon-based single-atom catalysts, as well their innovative applications mechanisms advanced oxidation technologies.

Language: Английский

---

Single Atoms and Clusters Based Nanomaterials for Hydrogen Evolution, Oxygen Evolution Reactions, and Full Water Splitting

Advanced Energy Materials, Journal Year: 2019, Volume and Issue: 9(22)

Published: May 2, 2019

Abstract The sustainable and scalable production of hydrogen through evolution reaction (HER) oxygen (OER) in water splitting demands efficient robust electrocatalysts. Currently, state‐of‐the‐art electrocatalysts Pt IrO 2 /RuO exhibit the benchmark catalytic activity toward HER OER, respectively. However, expanding their practical application is hindered by exorbitant price scarcity. Therefore, development alternative effective for crucial. In last few decades, substantial effort has been devoted to HER/OER catalysts based on various transition metals (including Fe, Co, Ni, Mo, atomic Pt) which show promising activities durability. this review, after a brief introduction basic mechanism HER/OER, authors systematically discuss recent progress design, synthesis, single atom cluster‐based catalysts. Moreover, crucial factors that can tune such as morphology, crystal defects, hybridization with nonmetals, heteroatom doping, alloying, formation inside graphitic layered materials are discussed. Finally, existing challenges future perspectives improving performance addressed.

Language: Английский

---

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

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: May 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

Language: Английский

---