近单位选择性乙烷非氧化脱氢制乙烯的光催化反应。

IF 15.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2025-10-23 DOI:10.1038/s41467-025-64389-9

Xiaoyu Sui,Jiwu Zhao,Pu Zhang,Ying Wang,Hangbin Zheng,Haihua Zeng,Pengzhao Wang,Yanyan Jia,Na Wen,Zhengxin Ding,Zizhong Zhang,Sheng Dai,Chao Xu,Rusheng Yuan,Wenxin Dai,Xianzhi Fu,Jinlin Long

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引用次数: 0

摘要

轻烷烃生成烯烃的非氧化脱氢反应在热力学上受到C-H键和C-C键断裂之间的权衡的限制。利用光催化解开热力学瓶颈，容易消除不良副反应，如深度脱氢、裂化、异构化和聚合。在此，我们展示了在环境条件下乙烷的非氧化脱氢，通过接枝Ni单原子来调节光沉积在锐钛矿型TiO2纳米颗粒表面的Pd纳米颗粒的表面电子结构，从而改变乙烷脱氢途径。在太阳光照下的流动反应器中，乙烷转化为乙烯和氢的速率高达8.2±0.2 mmol·g-1·h-1，乙烯选择性为100%。采用最佳的T-Ni0.6Pd0.24光催化剂，在350 nm处的表观量子效率达到~22.3%。太阳能驱动的非氧化烷烃脱氢为制备高性能、高选择性的轻质烯烃提供了一条途径。

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Photocatalytic non-oxidative dehydrogenation of ethane to ethene with near unit selectivity.

The non-oxidative dehydrogenation of light alkanes to alkenes is thermodynamically limited by the trade-off between the cleavage of C-H and C-C bonds. Unlocking the thermodynamic bottleneck with photocatalysis is prone to eliminate undesirable side reactions such as deep dehydrogenation, cracking, isomerization, and polymerization. Herein, we show the photocatalytic non-oxidative dehydrogenation of ethane to ethene and hydrogen at ambient conditions, which is enabled by grafting of Ni single atoms to modulate the surface electronic structure of Pd nanoparticles photo-deposited on the surface of anatase TiO2 nanoparticles, modifying the ethane dehydrogenation pathway. A high rate of 8.2 ± 0.2 mmol·g-1·h-1 for the stoichiometric conversion of ethane to ethene and hydrogen is achieved with a 100% ethene selectivity in a flow reactor under solar light irradiation. The apparent quantum efficiency reaches ~22.3% at 350 nm by using the optimal T-Ni0.6Pd0.24 photocatalyst. Solar-driven non-oxidative alkane dehydrogenation offers a route to light alkenes with high performance, and selectivity.

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.