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在电催化降低反应中确定动态活性位点

Yong Zhao^1,2, Shuang Gao³, Xiangyu Chen^1,2

¹State Key Laboratory of Bioinspired Interfacial Materials Science, Bioinspired Science Innovation Center, Hangzhou International Innovation Institute, Beihang University, Hangzhou 311115, China.

Journal of the American Chemical Society

|August 23, 2025

概括

无形氧化催化剂在酸盐降解过程中动态重组,产生高度活跃的氨产地. 这种操作成像揭示了缺陷的扩散,显著提高了催化性能.

科学领域:

电催化
材料科学
表面化学

背景情况:

了解反应条件下的催化剂演变对于设计高效的电催化剂至关重要.
传统技术难以将纳米级结构与催化活性联系起来,阻碍了催化剂设计.
酸盐还原反应 (NO3RR) 对于可持续的氨合成很重要.

研究的目的:

开发和应用一个集成的操作平台,同时进行纳米规模的地形和活动测绘.
在酸盐还原反应中研究无形SnO2的时空演变.
将结构变化与氨生产的局部催化活性相关联.

主要方法:

集成的电化学原子力显微镜 (EC-AFM) 和扫描电化学显微镜 (SECM).
在NO3RR过程中同时对表面地形和局部电流分布进行纳米级跟踪.
形态和晶体SnO2催化剂的形态分析和高度分析.

主要成果:

在催化过程中,无形SnO2催化剂表现出显著的表面重组和增加的粗度 (高达59.0%).
与基底平面相比,粗区域的氨 (NH3) 生产活动增加了约100倍.
无形催化剂显示出更大的厚度减小,并开发了具有Sn(II) 和Sn(0) 位点的双功能架构.

结论:

无形SnO2的电催化激活导致缺陷扩散,显著提高NH3产量.
开发的相关操作成像策略为研究短暂的催化动态提供了通用范式.
这种方法可以直接用于优化NO3RR和其他新出现的电催化过程.

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