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Au–Pd Tandem Photocatalysis for Nonoxidative Coupling of Methane toward Ethylene
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-05-01 , DOI: 10.1021/acscatal.3c00507
Chengyun Tang 1 , Shulin Du 1 , Haowei Huang 2 , Siyi Tan 1 , Jiwu Zhao 1 , Hongwen Zhang 2 , Wenkang Ni 1 , Xuanyu Yue 1 , Zhengxin Ding 1 , Zizhong Zhang 1 , Rusheng Yuan 1 , Wenxin Dai 1 , Xianzhi Fu 1 , Maarten B. J. Roeffaers 2 , Jinlin Long 1
Affiliation  

Photocatalytic nonoxidative coupling of CH4 to C2H4 with a high rate and selectivity is considered challenging and impractical due to complex chemical pathways and unfavorable thermodynamics. This work introduces a strategy of tandem photocatalysis based on Au and Pd nanoparticles codeposited on a Bi2NbO5F photocatalyst, which divides the CH4 to C2H4 reaction into two distinct steps carried out in tandem by multiple activity components, i.e., CH4 coupling to C2H6 on Au and C2H6 dehydrogenation on Pd. As a result, the optimized Au–Pd/Bi2NbO5F shows CH4 coupling to C2H4 with a high yield of 22.6 μmol g–1 h–1 and selectivity of 63% under simulated solar light irradiation. The reaction pathway is investigated by a series of activity experiments and in situ characterizations, demonstrating separate steps on Au and Pd. This work proposes a general strategy for the future design of photocatalysts to drive complex reactions efficiently and selectively based on the concept of a tandem system.

中文翻译:

Au-Pd 串联光催化甲烷非氧化偶联生成乙烯

由于复杂的化学途径和不利的热力学,以高速率和选择性将CH 4光催化非氧化偶联为 C 2 H 4被认为是具有挑战性和不切实际的。这项工作介绍了一种基于共沉积在 Bi 2 NbO 5 F 光催化剂上的 Au 和 Pd 纳米粒子的串联光催化策略,该策略将 CH 4转化为 C 2 H 4 的反应分为两个不同的步骤,由多个活性组分串联进行,即, CH 4偶联到Au 和C 2 H 6上的 C 2 H 6Pd 脱氢 因此,优化后的 Au–Pd/Bi 2 NbO 5 F 显示 CH 4与 C 2 H 4偶联,在模拟太阳光照射下具有 22.6 μmol g –1 h –1的高产率和 63% 的选择性。通过一系列活性实验和原位表征研究反应途径,展示 Au 和 Pd 上的独立步骤。这项工作提出了未来光催化剂设计的总体策略,以基于串联系统的概念高效和选择性地驱动复杂反应。
更新日期:2023-05-01
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