Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2021-04-24 , DOI: 10.1016/j.cej.2021.130016 Zhangqian Liang , Yanjun Xue , Xinyu Wang , Yanli Zhou , Xiaoli Zhang , Hongzhi Cui , Guiqing Cheng , Jian Tian
The Gibbs free energy of MoS2 for H+ absorption is near-zero, which is considered to be a promising cocatalyst for H2 production. Nevertheless, the activity of MoS2 for HER is greatly limited by the acidic environment. Herein, we study that Co-doped MoS2 (Co-MoS2) nanosheets can realize an extremely efficient photocatalytic H2 production of g-C3N4 nanosheet (NSs) in alkalescent environment, such as triethanolamine (TEOA). The optimized Co-MoS2/g-C3N4 hybrids exhibits extremely boosted photocatalytic H2 evolution rate of 3193 μmol-1 h-1 g-1, approximately 2.4, 6.0 and 42.0 times as much as MoS2/g-C3N4 (1326 μmol-1 h-1 g-1), CoS2/g-C3N4 (530 μmol-1 h-1 g-1) and pure g-C3N4 (76 μmol-1 h-1 g-1), respectively. Besides, we calculated the apparent quantum efficiency (AQE) of all photocatalysts under the light at λ=370 nm, and the AQE of Co-MoS2/g-C3N4 hybrids reaches 16.62%. DFT calculation and experimental data reveal that the outstanding HER activity of Co-MoS2/g-C3N4 hybrids is ascribed to the Co doping inducing the distortion of MoS2 crystal, which effectively reduces the H binding free energy for HER. The project of Co-MoS2/g-C3N4 hybrids provides experience on the progress of low-cost and highly effective photocatalysts for photocatalytic H2 evolution.
中文翻译:
Co掺杂的MoS 2作为助催化剂可显着改善碱性环境中gC 3 N 4的光催化氢析出
MoS 2吸收H +的吉布斯自由能接近于零,被认为是产生H 2的有前途的助催化剂。然而,MoS 2对HER的活性受到酸性环境的极大限制。在本文中,我们研究了共掺杂的MoS 2(Co-MoS 2)纳米片可以在碱性环境如三乙醇胺(TEOA)中实现gC 3 N 4纳米片(NSs)的非常高效的光催化H 2产生。优化的Co-MoS 2 / gC 3 N 4杂化物表现出极强的光催化H 2含量演化速率为3193μmol -1 h -1 g -1,约为MoS 2 / gC 3 N 4(1326μmol -1 h -1 g -1),CoS 2 / gC 3 N的2.4、6.0和42.0倍4(530μmol -1 h -1 g -1)和纯gC 3 N 4(76μmol -1 h -1 g -1), 分别。此外,我们计算了所有光催化剂在λ= 370 nm光下的表观量子效率(AQE),Co-MoS 2 / gC 3 N 4杂化体的AQE达到16.62%。DFT计算和实验数据表明,Co-MoS 2 / gC 3 N 4杂化物的优异HER活性归因于Co掺杂引起MoS 2晶体的畸变,从而有效降低了HER的H结合自由能。Co-MoS 2 / gC 3 N 4杂化项目为光催化H 2低成本和高效光催化剂的发展提供了经验 进化。