Nickel single-atom catalysts intrinsically promoted by fast pyrolysis for selective electroreduction of CO2 into CO

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2022-05-01 DOI:10.1016/j.apcatb.2021.120997

Yibo Guo , Sai Yao , Yuanyuan Xue , Xu Hu , Huijuan Cui , Zhen Zhou

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引用次数: 44

Abstract

The electrochemical reduction reaction of carbon dioxide (CO₂RR) is an effective way towards carbon neutralization. Single-atom catalysts (SACs) are expected to be efficient for CO₂RR due to maximum atom utilization and excellent catalytic performance. Here, nitrogen-doped carbon supported Ni SACs (Ni-SAC@NCs) were prepared through effective fast pyrolysis. CO₂ can convert into CO efficiently with Ni-SAC@NCs as electrocatalysts for CO₂RR. The faradaic efficiency kept well above 80% in the applied potential window of −0.6 to −0.9 V (vs. reversible hydrogen electrode (RHE)), with a highest FE_CO of 95% at −0.6 V (vs. RHE). Ni-SAC@NCs can achieve the best CO selectivity under a small overpotential, surpassing most other state-of-the-art catalysts. Computations also indicate that the unique defect-Ni-N₃ structure is the active site. This work not only provides a simple and promising new route for the preparation of SACs, but also proves the key role of the coordination environment in electrocatalysis.

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镍单原子快速热解催化剂选择性电还原CO2为CO

二氧化碳的电化学还原反应是实现碳中和的有效途径。单原子催化剂(SACs)由于其最大的原子利用率和优异的催化性能，有望成为高效的CO2RR催化剂。本文通过高效快速热解制备了氮掺杂碳负载Ni SACs (Ni-SAC@NCs)。Ni-SAC@NCs作为CO2RR的电催化剂，可以有效地将CO2转化为CO。在−0.6 ~−0.9 V(相对于可逆氢电极(RHE))的电位窗口内，法拉第效率保持在80%以上，在−0.6 V(相对于RHE)时最高的FECO为95%。Ni-SAC@NCs在过电位小的情况下可以达到最佳的CO选择性，超过大多数其他先进的催化剂。计算还表明，独特的缺陷- ni - n3结构是活性位点。这项工作不仅为SACs的制备提供了一条简单而有前途的新途径，而且证明了配位环境在电催化中的关键作用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.