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掺杂剂引发的原子结构可激活水分解为氢气。

Dopant triggered atomic configuration activates water splitting to hydrogen.

机构信息

Division of Nanomaterials & Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, New Cornerstone Science Laboratory, Department of Chemistry, Institute of Biomimetic Materials & Chemistry, Anhui Engineering Laboratory of Biomimetic Materials, University of Science and Technology of China, Hefei, 230026, Anhui, P. R. China.

Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, 215123, Suzhou, P. R. China.

出版信息

Nat Commun. 2023 Apr 21;14(1):2306. doi: 10.1038/s41467-023-37641-3.

DOI:10.1038/s41467-023-37641-3
PMID:37085504
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10121564/
Abstract

Finding highly efficient hydrogen evolution reaction (HER) catalysts is pertinent to the ultimate goal of transformation into a net-zero carbon emission society. The design principles for such HER catalysts lie in the well-known structure-property relationship, which guides the synthesis procedure that creates catalyst with target properties such as catalytic activity. Here we report a general strategy to synthesize 10 kinds of single-atom-doped CoSe-DETA (DETA = diethylenetriamine) nanobelts. By systematically analyzing these products, we demonstrate a volcano-shape correlation between HER activity and Co atomic configuration (ratio of Co-N bonds to Co-Se bonds). Specifically, Pb-CoSe-DETA catalyst reaches current density of 10 mA cm at 74 mV in acidic electrolyte (0.5 M HSO, pH ~0.35). This striking catalytic performance can be attributed to its optimized Co atomic configuration induced by single-atom doping.

摘要

寻找高效的析氢反应(HER)催化剂对于实现向净零碳排放社会转型的最终目标至关重要。此类 HER 催化剂的设计原则在于众所周知的结构-性质关系,该关系指导着合成程序,从而创造出具有催化活性等目标性质的催化剂。在这里,我们报告了一种合成 10 种单原子掺杂 CoSe-DETA(DETA=二乙三胺)纳米带的通用策略。通过系统地分析这些产物,我们证明了 HER 活性与 Co 原子构型(Co-N 键与 Co-Se 键的比例)之间存在火山形状的相关性。具体而言,在酸性电解质(0.5 M HSO,pH~0.35)中,Pb-CoSe-DETA 催化剂在 74 mV 时达到了 10 mA cm 的电流密度。这种显著的催化性能可归因于单原子掺杂诱导的优化的 Co 原子构型。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/7d9c97b915d2/41467_2023_37641_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/e42fca8a6158/41467_2023_37641_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/fd179e43ced4/41467_2023_37641_Fig2_HTML.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/817df6ed3179/41467_2023_37641_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/7d9c97b915d2/41467_2023_37641_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/e42fca8a6158/41467_2023_37641_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/fd179e43ced4/41467_2023_37641_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/4eb3a766ae51/41467_2023_37641_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/817df6ed3179/41467_2023_37641_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5f58/10121564/7d9c97b915d2/41467_2023_37641_Fig5_HTML.jpg

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