Pd single-atom decorated CdS nanocatalyst for highly efficient overall water splitting under simulated solar light
Pd single-atom decorated CdS nanocatalyst for highly efficient overall water splitting under simulated solar light
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Pd单原子修饰的CdS纳米催化剂可在模拟太阳光下实现高效的整体水分解
DOI：
10.1016/j.apcatb.2021.121000
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发表时间：
2022-05-01
影响因子：
22.1
通讯作者：
Wang, Chuan-yi
中科院分区：
文献类型：
--
作者：
Li, Wei;Chu, Xiao-shan;Wang, Chuan-yi
太阳能诱导的整体水分解制氢是对能源可持续性的鼓舞，但由于其有限的效率严重阻碍了其实际应用的规模，因此也是令人生畏的。CdS是一种重要的低功函数过渡金属硫化物。然而，其光稳定性往往由于光腐蚀的影响而恶化。为了克服这个问题，本文采用单原子Pd修饰CdS，通过简单可控的光诱导还原策略形成CdS-Pd纳米催化剂。协同半导体（CdS）-金属（Pd）相互作用促进了快速的体到表面电子迁移，从而所得的CdS-Pd（3.83ppm）纳米催化剂显示出相当大的结构稳定性和显著改善的太阳能诱导的HER活性，在整体水裂解中，比原始CdS高约110倍。同时，在420 nm/500 nm的光照射下，该修饰纳米催化剂的表观量子产率（AQY）分别为4.47%/1.81%和33.92%/27.49%，显示了在宽带光照射下的高效性.密度泛函理论（DFT）的计算结果表明，修饰后的纳米催化剂由于能垒较低，容易形成H* 中间体，这是内部促进的产氢机制.该研究为获得稳定的CdS基光催化剂提供了重要的见解，用于高效的整体水裂解制氢。
Solar-induced overall water splitting to produce hydrogen is inspiring towards energy sustainability, but it is also formidable due to its limited efficiency seriously hindering its scale up for practical application. CdS is an important transition metal sulfide with low-work-function. However, its photostability is often deteriorated due to photocorrosion influence. To overcome this issue, single-atom Pd was employed here to decorate CdS to form a CdS-Pd nanocatalyst through a simple and controllable photoinduced reduction strategy. The synergetic semiconductor (CdS)-metal (Pd) interaction promotes the fast bulk-to-surface electron migration, thereby the resultant CdS-Pd (3.83 parts per thousand) nanocatalyst shows considerable structural stability and dramatically improved solar induced HER activity in overall water splitting, about 110-fold higher than that of pristine CdS. Meanwhile, high apparent quantum yields (AQYs) of 4.47%/1.81% and 33.92%/27.49% were respectively achieved with this decorated nanocatalyst under the light of 420 nm/500 nm in absence and presence of scavenger, demonstrating the high-efficiency under broadband light illumination. Density functional theory (DFT) calculation supports that the easy formation of H* intermediates on the decorated nanocatalyst due to low energy barriers accounts for the internal promoted mechanism for hydrogen production. This study provides important insight to gain stable CdSbased photocatalysts for high-efficient hydrogen production by overall water splitting.