Insight into the synthesis of alcohols and acids in plasma-driven conversion of CO2 and CH4 over copper-based catalysts
Insight into the synthesis of alcohols and acids in plasma-driven conversion of CO2 and CH4 over copper-based catalysts
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深入了解铜基催化剂上等离子体驱动的 CO2 和 CH4 转化过程中醇和酸的合成
DOI：
10.1016/j.apcatb.2022.121583
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发表时间：
2022-06
影响因子：
22.1
通讯作者：
Li Wang
中科院分区：
文献类型：
--
作者：
Yuezhao Wang;Linhui Fan;Hongli Xu;Xiaomin Du;Haicheng Xiao;Ji Qian;Yimin Zhu;Xin Tu;Li Wang
在温和条件下将二氧化碳和甲烷直接转化为增值氧化物是非常可取的，因为它具有实现可持续低碳经济和碳中和生态系统的巨大潜力。然而，在这一过程中调整氧合物的分布仍然是一个主要的挑战。本研究利用铜基催化剂的电子结构和酸性特性作为策略，在反应温度为60℃、常压下调节CO 2和ch4等离子体催化转化过程中氧合物（醇类和酸类）的分布。我们使用锚定铜的载体来调节Cu 2+和Cu +在Cu基催化剂中的分布。综合表征和反应性能表明，Cu 2+有利于醇的生成，而Cu +对乙酸的生成至关重要。此外，HZSM-5的Brønsted酸位点显著提高了乙酸的选择性，而分离的Cu +中心和Brønsted酸位点的协同作用，通过Cu交换HZSM-5发展，具有形成乙酸的潜力。最后，讨论了醇和乙酸形成的可能途径。这项工作为高选择性催化剂的设计提供了新的见解，用于调节CO 2和CH 4在等离子体催化转化为氧合物中的醇和酸的分布。•研究了CO 2和ch4在cu基催化剂上的等离子体转化为氧合物。•可以通过调整Cu价态和催化剂酸度来定制含氧盐分布。•催化剂上cu2 +的存在对R-OH的形成至关重要。•Cu +物种和Brønsted酸位点都有助于R-COOH的生成。•铜和Brønsted酸位点的协同作用显示了形成R-COOH的潜力。
Direct conversion of CO 2 and CH 4 into value-added oxygenates under mild conditions is highly desirable since it has great potential to deliver a sustainable low-carbon economy and a carbon-neutral ecosystem. However, tuning the distribution of oxygenates in this process remains a major challenge. Here, the electronic structure and acidic properties of copper-based catalysts were exploited as strategies to tune the distribution of oxygenates (alcohols and acids) in the plasma-catalytic conversion of CO 2 and CH 4 at a reaction temperature of 60 °C and atmospheric pressure. We use support, on which copper is anchored, to regulate the distribution of Cu 2+ and Cu + in the Cu-based catalysts. Comprehensive characterization of the catalysts together with the reaction performances reveals that Cu 2+ species are favorable to the formation of alcohols, whereas Cu + species are critical to enhancing acetic acid production. Furthermore, the Brønsted acid sites of HZSM-5 significantly improved the selectivity of acetic acid, while the synergy of isolated Cu + center and Brønsted acid sites, developed via Cu-exchange HZSM-5, exhibits potential for acetic acid formation. Finally, possible pathways for the formation of alcohols and acetic acid have been discussed. This work provides new insights into the design of highly selective catalysts for tuning the distribution of alcohols and acids in the plasma-catalytic conversion of CO 2 and CH 4 to oxygenates. • Plasma conversion of CO 2 and CH 4 to oxygenates over Cu-based catalysts was studied. • Oxygenate distribution can be tailored by tuning Cu valence state and catalyst acidity. • The presence of Cu 2+ species on the catalysts is critical to forming R-OH. • Both Cu + species and the Brønsted acid site contribute to the generation of R-COOH. • The synergy of copper and Brønsted acid site shows the potential to form R-COOH.
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影响因子：
3.6
作者：
T. Kolb;Jan H. Voigt;K. Gericke
通讯作者：
T. Kolb;Jan H. Voigt;K. Gericke
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影响因子：
22.1
作者：
Diao, Yanan;Zhang, Xiao;Shi, Chuan
通讯作者：
Shi, Chuan
影响因子：
12.9
作者：
Wang, Li;Yi, Yanhui;Tu, Xin
通讯作者：
Tu, Xin
影响因子：
7.4
作者：
Krawczyk, K.;Mlotek, M.;Schmidt-Szalowski, K.
通讯作者：
Schmidt-Szalowski, K.
影响因子：
3.6
作者：
A. Rahmani;M. Nikravech
通讯作者：
A. Rahmani;M. Nikravech