Phosphorus-modified cobalt single-atom catalysts loaded on crosslinked carbon nanosheets for efficient alkaline hydrogen evolution reaction

Nanoscale, Journal Year: 2023, Volume and Issue: 15(7), P. 3550 - 3559

Published: Jan. 1, 2023

Efficient and low-cost transition metal single-atom catalysts (TMSACs) for hydrogen evolution reaction (HER) have been recognized as research hotspots recently with advances in delivering good catalytic activity without noble metals. However, the high-cost complex preparation of TMSACs insufficient stability limited their practical applications. Herein, a simple top-down pyrolysis approach to obtain P-modified Co SACs loaded on crosslinked defect-rich carbon nanosheets was introduced alkaline evolution, where atoms are locally confined before prevent aggregation. Thereby, abundant defects unsaturated coordination formed during significantly improved monatomic structure reduced barrier. Furthermore, synergy between cobalt phosphorus established optimize decomposition process water molecules, which delivers key promoting slow kinetics HER. As result, SAC exhibited excellent HER, overpotentials 70 mV 192 at current densities -10 mA cm-2 -100 cm-2, respectively.

Language: Английский

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Highly selective semiconductor photocatalysis for CO₂ reduction

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(24), P. 12539 - 12558

Published: Jan. 1, 2023

Herein, to provide ideas for the design of highly selective CO 2 reduction materials, we introduce each step photocatalytic process and summarize how is adjusted promote selectivity reduction.

Language: Английский

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Integrating Host Design and Tailored Electronic Effects of Yolk–Shell Zn−Mn Diatomic Sites for Efficient CO₂ Electroreduction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(3)

Published: Nov. 24, 2023

Abstract Modulating the surface and spatial structure of host is associated with reactivity active site, also enhances mass transfer effect CO 2 electroreduction process (CO RR). Herein, we describe development two‐step ligand etch–pyrolysis to access an asymmetric dual‐atomic‐site catalyst (DASC) composed a yolk–shell carbon framework (Zn 1 Mn ‐SNC) derived from S,N‐coordinated Zn−Mn dimers anchored on metal–organic (MOF). In Zn ‐SNC, electronic effects S/N−Zn−Mn−S/N configuration are tailored by strong interactions between dual sites co‐coordination S/N atoms, rendering structural stability atomic distribution. H‐cell, ‐SNC DASC shows low onset overpotential 50 mV high Faraday efficiency 97 % applied 343 mV, thus outperforming counterparts, in flow cell, it reaches current density 500 mA cm −2 at −0.85 V, benefitting accessibility sites. DFT simulations showed that diatomic site optimal adsorption strength COOH* lowers reaction energy barrier, boosting intrinsic RR activity DASC. The structure‐property correlation found this study suggests new ideas for highly accessible catalysts.

Language: Английский

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How to select heterogeneous CO ₂ reduction electrocatalyst

Deleted Journal, Journal Year: 2023, Volume and Issue: 3, P. e9120096 - e9120096

Published: Sept. 1, 2023

As an important part of carbon neutralization, dioxide electroreduction reaction (CO₂RR) can convert CO₂ into high value-added chemicals and fuels to realize the recycling resources solve problem environmental pollution. Therefore, exploring element species surface structure catalyst plays a central role in improving performance catalyst, enhancing conversion efficiency forming C₁ C₂₊ products. Here, we summarize recent progress selective regulation CO₂RR products by different elements. In particular, emphasize structure-property relationship microenvironment metal center substrate, heteroatom doping, hydrogen bond network metal-free polymer, construction heterogeneous catalytic system. At same time, advances for identification active sites mechanistic studies on process reducing are reviewed, as well comprehensive review final Finally, outline inevitable challenges faced present our own recommendations aimed at contributing resource utilization.

Language: Английский

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Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: July 11, 2023

Electrochemical carbon dioxide reduction reaction (CO2RR) provides a promising way to convert CO2 chemicals. The multicarbon (C2+) products, especially ethylene, are of great interest due their versatile industrial applications. However, selectively reducing ethylene is still challenging as the additional energy required for C-C coupling step results in large overpotential and many competing products. Nonetheless, mechanistic understanding key steps preferred pathways/conditions, well rational design novel catalysts production have been regarded approaches achieving highly efficient selective CO2RR. In this review, we first illustrate CO2RR (e.g., adsorption/activation, formation *CO intermediate, step), offering conversion ethylene. Then alternative pathways conditions competitive products (C1 other C2+ products) investigated, guiding further development generation. Engineering strategies Cu-based CO2RR-ethylene summarized, correlations mechanism/pathways, engineering selectivity elaborated. Finally, major challenges perspectives research area proposed future practical

Language: Английский

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Advanced electrocatalytic technologies for conversion of carbon dioxide into methanol by electrochemical reduction: Recent progress and future perspectives

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 482, P. 215081 - 215081

Published: Feb. 28, 2023

Language: Английский

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In Situ/Operando Methods for Understanding Electrocatalytic Nitrate Reduction Reaction

Small Methods, Journal Year: 2023, Volume and Issue: 7(7)

Published: April 10, 2023

With the development of industrial and agricultural, a large amount nitrate is produced, which not only disrupts natural nitrogen cycle, but also endangers public health. Among commonly used treatment techniques, electrochemical reduction reaction (eNRR) has attracted extensive attention due to its mild conditions, pollution-free nature, other advantages. An in-depth understanding eNRR mechanism prerequisite for designing highly efficient electrocatalysts. However, some traditional characterization tools cannot comprehensively deeply study process. It necessary develop in situ operando techniques reveal at time-resolved atomic level. This review discusses summarizes possible eNRR. A detailed introduction various their help provided. Finally, current challenges future opportunities this research area are discussed highlighted.

Language: Английский

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Controllable synthesis of high-entropy alloys

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(12), P. 6021 - 6041

Published: Jan. 1, 2024

This review provides a comprehensive overview of the recent advancements in controllable synthesis high-entropy alloys, ranging from approach and significance composition, morphology, structure, surface/interface engineering.

Language: Английский

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Electronic engineering and oxygen vacancy modification of La_0.6Sr_0.4FeO_3−δ perovskite oxide by low-electronegativity sodium substitution for efficient CO₂/CO fueled reversible solid oxide cells

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(6), P. 3202 - 3210

Published: Jan. 1, 2024

Sodium doping increases oxygen vacancy concentration, modulates the electronic structure, and improves CO 2 chemical adsorption, enabling superior /CO reversible conversion.

Language: Английский

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Opening Direct Electrochemical Fischer–Tropsch Synthesis Path by Interfacial Engineering of Cu Electrode with P-Block Elements

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(3), P. 3368 - 3387

Published: Jan. 12, 2024

The electrochemical synthesis of syngas (CO and H2) has garnered considerable attention in the context Fischer–Tropsch (FT) employing thermal catalysts. Nonetheless, need for a novel, cost-effective technique persists. In this investigation, we introduce direct (dEC) approach FT that functions under ambient conditions by utilizing p-block element (Sn In) overlaid Cu electrode. Surface *CO H* species were obtained an electrolytic medium through CO2 + H+ e– → HOOCad (or CO adsorption) reactions, respectively. We have observed C2–7 long-chain hydrocarbons with CnH2n+2/CnH2n ratio 1–3, observation can be explained process C–C coupling chain growth conventional synthesis, based on linearity Anderson-Schulz–Flory equation plots. Thick Sn overlayers resulted dominant production formate, while C2H4 found to proportional inversely correlated H2, C2H6, C3–7 hydrocarbon production. EC CO2/CO reduction used dEC offers valuable insights into mechanism C2+ holds promise as eco-friendly producing energy environmental purposes.

Language: Английский

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