Enhanced Solar Fuel H-2 Generation over g-C3N4 Nanosheet Photocatalysts by the Synergetic Effect of Noble Metal-Free Co2P Cocatalyst and the Environmental Phosphorylation Strategy
Enhanced Solar Fuel H-2 Generation over g-C3N4 Nanosheet Photocatalysts by the Synergetic Effect of Noble Metal-Free Co2P Cocatalyst and the Environmental Phosphorylation Strategy
复制标题
通过无贵金属 Co2P 助催化剂的协同效应和环境磷酸化策略增强 g-C3N4 纳米片光催化剂上太阳能燃料 H-2 的生成
DOI：
10.1021/acssuschemeng.7b03169
复制
发表时间：
2018
影响因子：
8.4
通讯作者：
Li Xin
中科院分区：
文献类型：
--
作者：
Shen Rongchen;Xie Jun;Zhang Hongdan;Zhang Aiping;Chen Xiaobo;Li Xin
在开发实用的析氢反应(HER)系统方面，人们对高活性和耐用的富含地球的助催化剂和光催化剂的需求越来越大。特别是，开发不含贵金属的铂类助催化剂仍然是一个巨大的挑战。在这项研究中，深入研究和揭示了金属有机骨架(MOF)衍生的富稀土Co2P助催化剂和强大的生物启发的环境磷酸化策略在促进石墨化碳氮化物(g-C3N4)纳米片光催化生成H_2方面的协同效应。G-C3N4-Co2P-K2HPO4光催化体系的最大析氢速率可达27.81mol.h-1，约为纯g-C3N4纳米片的556倍。负载地球的Co2P纳米粒子具有良好的导电性，不仅可以提高可见光的吸收，减少电子-空穴对的复合，而且主要作为一种有效的助催化剂来降低析氢过电位。此外，K2HPO4可以通过质子还原循环产生额外的析氢途径，并通过有效地消耗空穴来增强TEOA的氧化能力，从而显著促进二元g-C3N4-Co2P异质结的光催化析氢。可以预见，这项工作将为合理制备无贵金属、低成本、高活性的金属磷化物共催化剂开辟一条新的途径，用于可见光照射下g-C3N4纳米片状光催化剂上高效的光催化析氢。
Highly active and durable earth-abundant cocatalysts and photocatalysts are under increasing demand in developing practical hydrogen-evolution reaction (HER) systems. Especially, exploiting noble-metal-free Pt-like HER cocatalysts still remains a significant challenge. In this study, the synergistic effect of metal–organic framework (MOF) derived earth-abundant Co2P cocatalysts and the robust bioinspired environmental phosphorylation strategy in boosting photocatalyic H2generation over the graphitic carbon nitride (g-C3N4) nanosheets was thoroughly investigated and revealed. The maximum H2-evolution rate of the ternary g-C3N4-Co2P-K2HPO4photocatalytic systems could reach 27.81 μmol h–1, which was approximately 556 times higher than that of pure g-C3N4nanosheets. The loaded earth-abundant Co2P nanoparticles with a good electrical conductivity could not only improve visible-light absorption and decrease the recombination of the electron–hole pairs, but also mainly serve as an efficient cocatalyst to lower the H2-evolution overpotentials. Furthermore, K2HPO4could generate an additional H2-evolution pathway through proton-reduction cycle and enhance the oxidation ability of TEOA by effectively consuming the holes, thus significantly boosting photocatalytic hydrogen evolution of the binary g-C3N4-Co2P heterojunctions. It could be anticipated that this work will open a new pathway to rationally fabricate a noble metal-free, low-cost and high-activity metal phosphide cocatalyst for efficient photocatalytic hydrogen evolution over g-C3N4nanosheet photocatalysts under visible-light illumination.