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Efficient photocatalytic hydrogen evolution over carbon supported antiperovskite cobalt zinc nitride
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-10-12 , DOI: 10.1016/j.cej.2020.127307
Siqi Liu , Xiangjian Meng , Samira Adimi , Haichuan Guo , Weiliang Qi , J. Paul Attfield , Minghui Yang

Photocatalytic solar to chemical energy conversion is an important energy conversion process but suffer from low efficiency. Thus, development of efficient photocatalytic system using earth-abundant elements with low costs is highly desirable. Here, antiperovskite cobalt zinc nitride has been synthesized and coupled with carbon black (Co3ZnN/C) for visible light driven hydrogen production in an Eosin Y-sensitized system. Replacement of cobalt atom by zinc atom leads to an improved charge transfer kinetics and catalytic properties compared with Co4N. Density functional theory (DFT) calculations further reveal the adjusted electronic structure of Co3ZnN by zinc atom introducing. The lower antibonding energy states of Co3ZnN are beneficial for the hydrogen desorption. Moreover, carbon black as support effectively reduces the particle size of Co3ZnN and benefits to the electron storage and adsorption capabilities. The optimal Co3ZnN/C catalysts exhibit the H2 evolution rate of 15.4 μmol mg-1 h-1, which is over 6 times higher than that of monometallic Co4N. It is even greater than those of most of Eosin Y-sensitized systems.



中文翻译:

碳载钙钛矿型钴锌氮化物的高效光催化制氢

光催化太阳能到化学能的转换是重要的能量转换过程,但是效率低下。因此,非常需要开发使用低成本的富含地球的元素的有效的光催化系统。在这里,已经合成了抗钙钛矿型钴锌氮化锌,并与炭黑(Co 3 ZnN / C)偶联,用于在曙红Y敏化系统中产生可见光,驱动氢的产生。与Co 4 N相比,用锌原子取代钴原子可改善电荷转移动力学和催化性能。密度泛函理论(DFT)计算进一步揭示了通过引入锌原子可调节Co 3 ZnN的电子结构。Co 3的较低抗键能态ZnN对于氢解吸是有益的。此外,作为载体的炭黑有效地减小了Co 3 ZnN的粒径,并有利于电子存储和吸附能力。最佳的Co 3 ZnN / C催化剂的H 2释放速率为15.4μmolmg -1 h -1,是单金属Co 4 N的H 2释放速率的6倍以上。甚至比大多数曙红Y-的高。敏化系统。

更新日期:2020-10-13
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