在化学合成、能源转化和环境修复等领域，纳米催化剂起着至关重要的作用。然而，对于金属/金属氧化物纳米催化剂来说，在还原气氛下金属的价态会发生动态变化，这使得它们的结构敏感性变得模糊不清。有研究聚焦于锰（Mn）基纳米催化剂。研究人员进行了一项测试反应，将可持续合成气转化为芳烃，这个过程对催化剂的氧化还原环境和活性位点特性高度敏感。研究深入分析了结构 - 活性关系（SAR），发现萨巴捷效应、一氧化碳（CO）吸附与芳烃的时空产率之间存在直接关联。结果表明，处于 +2 氧化态的锰是实现最高催化性能的最佳价态，芳烃的最大产率可达 1.6 毫摩尔每小时每克催化剂。这项研究成果为理解催化剂固有性质在一氧化碳加氢反应中的选择性和效率方面提供了关键见解，有助于合理设计纳米催化剂，将小分子可持续地转化为有价值的化学品和燃料。
期刊
Journal of the American Chemical Society
标题
Determination of Mn Valence States in Nanocatalysts During Sustainable Syngas Conversion
作者
Zhiping Li, Duohua Liao, Guo Tian, Xiaoyu Fan, Xu Chai, Wenxi Chang, Yuan Gao, Bo Yuan, Zonglong L, Fei Wei, Chenxi Zhang
摘要
Constructing structure–activity relationships (SAR) between nanocatalysts under reactive atmospheres makes them indispensable for chemical synthesis, energy transformation, and environmental remediation. However, this structure sensitivity remains ambiguous for metals/metal oxides due to dynamic changes in metal valences under a reductive atmosphere. Herein, this study delves into the complexities of Mn-based nanocatalysts, focusing on the impact of the Mn valence state in a test reaction converting sustainable syngas to aromatics-a process highly sensitive to the catalyst’s redox environment and active site characteristics. We conducted a thorough SAR analysis and discovered a direct correlation between the Sabatier effect, CO adsorption, and the space-time yields of aromatics. Notably, Mn in the +2-oxidation state emerged as the optimal valence for achieving the highest catalytic performance, with a maximum yield of 1.6 mmol·h–1·gcat–1. Our findings provide critical insights into the role of the catalyst’s intrinsic properties in dictating the selectivity and efficiency of CO hydrogenation for the rational design of nanocatalysts that can sustainably transform small molecules into valuable chemicals and fuels.
原文链接
https://pubs.acs.org/doi/10.1021/jacs.5c06550
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静远嘲风（MY Scimage） 成立于2007年，嘲风取自中国传统文化中龙生九子，子子不同的传说，嘲风为守护屋脊之瑞兽，喜登高望远；静远取自成语“宁静致远”，登高莫忘初心，远观而不可务远。
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