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Enhanced visible light photocatalytic non-oxygen coupling of amines to imines integrated with hydrogen production over Ni/CdS nanoparticles†
Catalysis Science & Technology ( IF 5 ) Pub Date : 2018-08-16 00:00:00 , DOI: 10.1039/c8cy01326h
Weiwei Yu 1, 2, 3, 4, 5 , Di Zhang 1, 2, 3, 4, 5 , Xinwen Guo 1, 2, 3, 4, 5 , Chunshan Song 1, 2, 3, 4, 5 , Zhongkui Zhao 1, 2, 3, 4, 5
Affiliation  

This work presents an efficient strategy for visible light-driven imine production through a photocatalytic non-oxygen coupling reaction of diverse amines dramatically boosted by hydrogen evolution over noble metal-free Ni/CdS nanoparticles. Thanks to the integrating effect, close to 100% conversion of benzylamine (75.2 h−1 turnover frequency), 97% selectivity for imine with 21.4 mmol g−1 h−1 hydrogen evolution rate (λ > 420 nm) and 11.2% apparent quantum yield (450 nm, 10 mg catalyst) have been achieved at room temperature and ambient pressure. In comparison with the use of common sacrificial agents like TEOA or Na2S/Na2SO3, by the coupling of amines to imines, the H2 evolution rate increases by two orders of magnitude. The aforementioned integrating strategy has been extended to diverse amines, and an outstanding photocatalytic performance for H2 and imine production was obtained. Besides, the catalyst can be recycled several times without evident activity loss, suggesting a bright prospect for sustainable chemistry and solar utilization. This new discovery may open a new horizon for efficiently boosting solar hydrogen evolution and simultaneously clean producing diverse high value-added fine chemicals under mild conditions.

中文翻译:

Ni / CdS纳米粒子上胺与亚胺的可见光增强光催化非氧偶联并产生氢气

这项工作提出了一种有效的策略,通过各种胺的光催化非氧偶联反应,通过可见光驱动的亚胺生产,该反应通过氢气的释放大大促进了不含贵金属的Ni / CdS纳米粒子的氢生成。由于积分效应,苄胺的转化率接近100%(75.2 h -1转换频率),对亚胺的选择性为97%,析氢速率为21.4 mmol g -1 h -1λ > 420 nm),表观量子为11.2%在室温和环境压力下已获得产率(450 nm,10 mg催化剂)。与使用常见的牺牲剂(例如TEOA或Na 2 S / Na 2 SO 3)相比通过将胺与亚胺偶联,H 2的析出速率提高了两个数量级。前述的整合策略已经扩展到多种胺,并且获得了对于H 2和亚胺生产的出色的光催化性能。此外,该催化剂可以循环使用几次而不会明显损失活性,这为可持续的化学和太阳能利用提供了广阔的前景。这一新发现可能为在温和条件下有效促进太阳能氢的释放并同时清洁生产各种高附加值精细化学品开辟新的视野。
更新日期:2018-08-16
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