Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(36), P. 19572 - 19590

Published: Feb. 19, 2021

Abstract Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy convert renewable feedstocks energy sources into transportable fuels value‐added chemicals. A crucial step in conducting e‐refinery processes development of appropriate reactions optimal electrocatalysts for efficient cleavage formation chemical bonds. However, compared well‐studied primary (e.g., O 2 reduction, water splitting), mechanistic aspects materials design complex are yet be settled. To address this challenge, herein, we first present fundamentals heterogeneous electrocatalysis some reactions, then implement these establish framework by coupling situ generated intermediates (integrated reactions) or products (tandem reactions). We also set principles strategies efficiently manipulate reaction pathways.

Language: Английский

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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

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Artificial channels for confined mass transport at the sub-nanometre scale

Nature Reviews Materials, Journal Year: 2021, Volume and Issue: 6(4), P. 294 - 312

Published: Jan. 21, 2021

Language: Английский

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Water decontamination via nonradical process by nanoconfined Fenton-like catalysts

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: May 19, 2023

Abstract There is an urgent need to develop effective and sustainable solutions reduce water pollution. Heterogeneous Fenton-like catalysts are frequently used eliminate contaminants from water. However, the applicability of these limited due low availability reactive species (RS). Herein, nanoconfinement strategy was applied encapsulate short-lived RS at nanoscale boost utilization efficiency in reactions. The nanoconfined catalyst fabricated by assembling Co 3 O 4 nanoparticles carbon nanotube nanochannels achieve exceptional reaction rate excellent selectivity. Experiments collectively suggested that degradation attributed singlet oxygen ( 1 2 ). Density functional theory calculations demonstrated space contributes quantum mutation alters transition state lower activation energy barriers. Simulation results revealed enrichment contaminant on reduced migration distance enhanced . synergy between shell layer core-shell structure further improved selectivity towards oxidation real waters. expected provide a viable for pollution control.

Language: Английский

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Designing Sites in Heterogeneous Catalysis: Are We Reaching Selectivities Competitive With Those of Homogeneous Catalysts?

Chemical Reviews, Journal Year: 2022, Volume and Issue: 122(9), P. 8594 - 8757

Published: March 3, 2022

A critical review of different prominent nanotechnologies adapted to catalysis is provided, with focus on how they contribute the improvement selectivity in heterogeneous catalysis. Ways modify catalytic sites range from use reversible or irreversible adsorption molecular modifiers immobilization tethering homogeneous catalysts and development well-defined solid surfaces. The latter covers methods for dispersion single-atom within supports as well complex nanostructures, it includes post-modification materials via processes such silylation atomic layer deposition. All these methodologies exhibit both advantages limitations, but all offer new avenues design specific applications. Because high cost most fact that resulting may limited thermal chemical stability, be best aimed at improving selective synthesis value-added chemicals, incorporated organic schemes, other applications are being explored address problems energy production, instance, greener processes. details each approaches discussed, representative examples provided. We conclude some general remarks future this field.

Language: Английский

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Atomically dispersed Ni species on N-doped carbon nanotubes for electroreduction of CO2 with nearly 100% CO selectivity

Applied Catalysis B Environment and Energy, Journal Year: 2020, Volume and Issue: 271, P. 118929 - 118929

Published: March 28, 2020

Language: Английский

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Size‐Dependent Activity and Selectivity of Atomic‐Level Copper Nanoclusters during CO/CO₂ Electroreduction

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 60(1), P. 466 - 472

Published: Sept. 18, 2020

Abstract As a favorite descriptor, the size effect of Cu‐based catalysts has been regularly utilized for activity and selectivity regulation toward CO 2 /CO electroreduction reactions (CO /CORR). However, little progress made in regulating Cu nanoclusters at atomic level. Herein, size‐gradient from single atoms (SAs) to subnanometric clusters (SCs, 0.5–1 nm) (NCs, 1–1.5 on graphdiyne matrix are readily prepared via an acetylenic‐bond‐directed site‐trapping approach. Electrocatalytic measurements show significant both /CORR. Increasing will improve catalytic C 2+ productions CORR. A high conversion rate 312 mA cm −2 with Faradaic efficiency 91.2 % achieved −1.0 V versus reversible hydrogen electrode (RHE) over NCs. The activity/selectivity‐size relations provide clear understanding mechanisms /CORR

Language: Английский

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Noble-Metal-Free Multicomponent Nanointegration for Sustainable Energy Conversion

Chemical Reviews, Journal Year: 2021, Volume and Issue: 121(17), P. 10271 - 10366

Published: July 6, 2021

Global energy and environmental crises are among the most pressing challenges facing humankind. To overcome these challenges, recent years have seen an upsurge of interest in development production renewable chemical fuels as alternatives to nonrenewable high-polluting fossil fuels. Photocatalysis, photoelectrocatalysis, electrocatalysis provide promising avenues for sustainable conversion. Single- dual-component catalytic systems based on nanomaterials been intensively studied decades, but their intrinsic weaknesses hamper practical applications. Multicomponent nanomaterial-based systems, consisting three or more components with at least one component nanoscale, recently emerged. The multiple integrated together create synergistic effects hence limitation outperformance. Such higher-efficiency will potentially bring additional benefit balance-of-system costs if they exclude use noble metals, considering expense sustainability. It is therefore timely review research this field, providing guidance noble-metal-free multicomponent nanointegration In work, we first recall fundamentals catalysis by nanomaterials, nanointegration, reactor configuration water splitting, CO2 reduction, N2 reduction. We then systematically discuss advances multicomponent-based photocatalytic, photoelectrochemical, electrochemical nanomaterials. On basis further laterally evaluate different integration strategies highlight impacts activity, performance stability, product selectivity. Finally, conclusions future prospects nanointegration. This work offers comprehensive insights into cost-competitive energy-conversion technologies assists researchers working toward addressing global environment.

Language: Английский

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Design of the Synergistic Rectifying Interfaces in Mott–Schottky Catalysts

Chemical Reviews, Journal Year: 2022, Volume and Issue: 123(1), P. 1 - 30

Published: Nov. 7, 2022

The functions of interfacial synergy in heterojunction catalysts are diverse and powerful, providing a route to solve many difficulties energy conversion organic synthesis. Among heterojunction-based catalysts, the Mott–Schottky composed metal–semiconductor with predictable designable rising stars next-generation catalysts. We review concept discuss their applications various realms catalysis. In particular, design catalyst provides feasible strategy boost chemical synthesis processes, even allowing realization novel catalytic such as enhanced redox activity, Lewis acid–base pairs, electron donor–acceptor couples for dealing current problems catalysis storage. This focuses on synthesis, assembly, characterization Schottky heterojunctions photocatalysis, electrocatalysis, proposed principles, including importance constructing stable clean interfaces, tuning work function differences, preparing exposable structures designing electronic will provide reference development all heterojunction-type electrodes, conversion/storage devices, super absorbers, which currently topics interest fields fuel cells, CO2 reduction, wastewater treatment.

Language: Английский

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2D Materials Bridging Experiments and Computations for Electro/Photocatalysis

Advanced Energy Materials, Journal Year: 2021, Volume and Issue: 12(4)

Published: Feb. 22, 2021

Abstract The exploration of catalysts for energy conversion lies at the center sustainable development. combination experimental and computational approaches can provide insights into inner laws between catalytic performance structural electronic properties catalysts. Owing to inherent advantages 2D materials over their 3D counterparts, including high specific surface area abundant defects that could sufficient active sites, are promising candidates have attracted wide interest in catalysis. Importantly, most widely computationally investigated models with which relate prediction confirmation conveniently. Recently, more been prepared experiments while accurate methods used disclose performance, explore mechanism an atomic level. In this review, recent advances summarized related development design electro/photocatalysts. main emphasis is put on unique by computations. Computational closer environments introduced particular attention bridge gap addition, challenges computations also discussed

Language: Английский

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