可持续合成气转化过程中纳米催化剂中Mn价态的测定

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Zhiping Li, Duohua Liao, Guo Tian*, Xiaoyu Fan, Xu Chai, Wenxi Chang, Yuan Gao, Bo Yuan, Zonglong Li, Fei Wei and Chenxi Zhang*, 
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引用次数: 0

摘要

在反应气氛下建立纳米催化剂之间的构效关系(SAR)使得纳米催化剂在化学合成、能量转化和环境修复中不可或缺。然而,由于还原气氛下金属价的动态变化,金属/金属氧化物的结构敏感性仍然不明确。在此,本研究深入研究了锰基纳米催化剂的复杂性,重点研究了锰价态在将可持续合成气转化为芳烃的测试反应中的影响——这一过程对催化剂的氧化还原环境和活性位点特征高度敏感。我们进行了全面的SAR分析,发现了萨巴蒂尔效应、CO吸附和芳烃时空产率之间的直接关系。值得注意的是,Mn的+2氧化态是达到最高催化性能的最佳价态,最大产率为1.6 mmol·h-1·gcat-1。我们的发现为催化剂的内在性质在决定CO加氢的选择性和效率方面的作用提供了重要的见解,为合理设计纳米催化剂提供了重要的见解,这些纳米催化剂可以持续地将小分子转化为有价值的化学品和燃料。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Determination of Mn Valence States in Nanocatalysts During Sustainable Syngas Conversion

Determination of Mn Valence States in Nanocatalysts During Sustainable Syngas Conversion

Determination of Mn Valence States in Nanocatalysts During Sustainable Syngas Conversion

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.

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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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