Design of Palladium-Doped g-C3N4 for Enhanced Photocatalytic Activity toward Hydrogen Evolution Reaction
Design of Palladium-Doped g-C3N4 for Enhanced Photocatalytic Activity toward Hydrogen Evolution Reaction
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钯掺杂 g-C3N4 增强析氢反应光催化活性的设计
DOI：
10.1021/acsaem.8b00526
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发表时间：
2018-05
影响因子：
6.4
通讯作者：
Ruibin Jiang
中科院分区：
文献类型：
--
作者：
Nan Wang;Jing Wang;Jinhui Hu;Xiaoqing Lu;Jie Sun;Feng Shi;Zong-Huai Liu;Zhibin Lei;Ruibin Jiang
石墨碳氮化物（g-C3 N4）具有良好的带隙和带边，被认为是一种很有前途的水分解光催化剂。但是，C_3N_4的析氢动力学非常缓慢。通常需要助催化剂来改善催化动力学。本文中，钯掺杂石墨碳氮化物（g-C3 N4-Pd）是利用Pd原子与-C3 N4六重腔的吡啶氮原子的牢固配位而设计的。Pd的引入并不影响g-C3 N4的结构和形貌。在-C_3N_4-Pd催化剂中，Pd以Pd离子形式存在，g-C_3 N_4-Pd催化剂的析氢活性明显高于-C_3N_4催化剂。Pd-C_3N_4的最高放氢活性是g-C_3 N_4的15.3倍。发现析氢活性的提高是由于电子激发方式的改变和Pd掺杂引起的析氢动力学的加速。我们的研究结果提供了一个很有前途的方法，以提高光催化析氢性能，并为开发高效和成本效益的光催化剂分解水铺平了新的途径。
Graphitic carbon nitride (g-C3N4) has been believed to be a promising photocatalyst for water splitting due to its right band gap and band edges. However, the kinetics of hydrogen evolution ong-C3N4is very slow. Cocatalysts are usually needed to improve the catalytic kinetics. Herein, palladium-doped graphitic carbon nitride (g-C3N4–Pd) is designed by virtue of the tenacious coordination of Pd atoms with the pyridinic nitrogen atoms of six-fold cavities ing-C3N4. The introduction of Pd does not affect the structure and morphology ofg-C3N4. Palladium is found to exist as Pd ions ing-C3N4–Pd catalysts.g-C3N4–Pd catalysts exhibit clearly higher hydrogen evolution activities thang-C3N4. The highest hydrogen evolution activity ong-C3N4–Pd is 15.3 times that ofg-C3N4. The improvement of hydrogen evolution activity is found to arise from both the alternation of the electron excitation manner and the acceleration of hydrogen evolution kinetics induced by Pd doping. Our findings provide a promising way to improve the photocatalytic performance for hydrogen evolution and pave a new avenue for the development of highly efficient and cost-effective photocatalysts for water splitting.