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Electrons and Hydroxyl Radicals Synergistically Boost the Catalytic Hydrogen Evolution from Ammonia Borane over Single Nickel Phosphides under Visible Light Irradiation.
ChemistryOpen ( IF 2.5 ) Pub Date : 2020-03-20 , DOI: 10.1002/open.201900335
Jin Song 1, 2 , Xiaojun Gu 1 , Hao Zhang 1
Affiliation  

From the perspective of tailoring the reaction pathways of photogenerated charge carriers and intermediates to remarkably enhance the solar‐to‐hydrogen energy conversion efficiency, we synthesized the three low‐cost semiconducting nickel phosphides Ni2P, Ni12P5 and Ni3P, which singly catalyzed the hydrogen evolution from ammonia borane (NH3BH3) in the alkaline aqueous solution under visible light irradiation at 298 K. The systematic investigations showed that all the catalysts had higher activities under visible light irradiation than in the dark and Ni2P had the highest photocatalytic activity with the initial turnover frequency (TOF) value of 82.7 min−1, which exceeded the values of reported metal phosphides at 298 K. The enhanced activities of nickel phosphides were attributed to the visible‐light‐driven synergistic effect of photogenerated electrons (e) and hydroxyl radicals (.OH), which came from the oxidation of hydroxide anions by photogenerated holes. This was verified by the fluorescent spectra and the capture experiments of photogenerated electrons and holes as well as hydroxyl radicals in the catalytic hydrogen evolution process.

中文翻译:

在可见光照射下,电子和羟基自由基协同促进单磷化镍上氨硼烷的催化氢释放。

从调整光生电荷载体和中间体的反应途径以显着提高太阳能到氢能的转化效率的角度出发,我们合成了三种低成本的半导体磷化镍Ni 2 P,Ni 12 P 5和Ni 3 P,在298 K可见光下单独催化碱性水溶液中氨硼烷(NH 3 BH 3)析氢。系统研究表明,所有催化剂在可见光照射下的活性均高于暗和Ni 2 P具有最高的光催化活性,初始转换频率(TOF)值为82.7分钟-1,超过报告的金属磷化物的值在298K增强镍磷化物的活性归因于光生电子(e的可见光驱动协同作用- )(和羟基自由基 OH),其从传来光生空穴氧化氢氧根阴离子 荧光光谱以及光催化电子放出过程中光生电子和空穴以及羟基自由基的捕获实验证实了这一点。
更新日期:2020-03-20
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