Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-09-23 , DOI: 10.1016/j.cej.2022.139378 Zhuogen Li , Gangqiang Zhu , Weibin Zhang , Lujun Zhu , Baowei Cao , Jianzhi Gao , Xianjin Shi , Yu Huang , Peng Liu , Mirabbos Hojamberdiev
In recent years, metal–semiconductor heterojunctions have been intensively researched in the field of photocatalysis due to the effective spatial separation of photo-induced electron-hole pairs. Here, the dual-functional copper (Cu0/Cu2+)-modified SrTiO3-δ nanosheets (Cu/STCO) are successfully synthesized by a two-step route. First, Cu2+-doped SrTiO3-δ (STCO) nanosheets are synthesized by a hydrothermal method and then Cu0 nanoparticles (NPs) are in situ formed from the STCO under H2 atmosphere at 500 °C. The optimized ratio 6 %-Cu/STCO photocatalyst exhibits the best photothermal catalytic performance for CO2 reduction reaction (CO2RR) and H2 evolution performance. The detailed characterization demonstrate that the Cu2+ dopant extend the light absorption range and the in situ generated Cu0 NPs effectively improve the separation ability of photogenerated charge carriers by forming the Schottky contact with STCO. The excited localized surface plasmon resonance (LSPR) effect of metallic Cu0 in Cu/STCO shows a considerable catalysis performance even under 600 nm monochromatic light irradiation. The density functional theory (DFT) calculations suggest that the Cu/STCO diminishes the barrier of the rate-determining steps of the CO2RR and H2 evolution thus perform the outstanding catalysis ability in two filed. This work presents the synergistic effect of Cu0 and Cu2+ on enhancing the photothermal catalytic performance for CO2RR and H2 evolution and offers a novel strategy to synthesize the metal–semiconductor nanostructures for efficient harnessing of solar energy into fuel.
中文翻译:
双功能铜 (Cu0/Cu2+) 改性 SrTiO3-δ 纳米片具有增强的光热催化 CO2 还原和 H2 释放性能
近年来,由于光生电子-空穴对的有效空间分离,金属-半导体异质结在光催化领域得到了深入研究。在这里,双功能铜(Cu 0 /Cu 2+)修饰的SrTiO 3-δ纳米片(Cu/STCO)通过两步法成功合成。首先,通过水热法合成Cu 2+掺杂的SrTiO 3-δ (STCO)纳米片,然后在500℃的H 2气氛下由STCO原位形成Cu 0纳米颗粒(NPs)。优化后的 6%-Cu/STCO 光催化剂对 CO 2表现出最佳的光热催化性能还原反应(CO 2 RR)和H 2释放性能。详细表征表明,Cu 2+掺杂剂扩展了光吸收范围,并且原位产生的Cu 0 NPs通过与STCO形成肖特基接触,有效地提高了光生电荷载流子的分离能力。即使在600 nm单色光照射下,金属Cu 0在Cu/STCO中的激发局部表面等离子体共振(LSPR)效应也显示出相当大的催化性能。密度泛函理论 (DFT) 计算表明,Cu/STCO 降低了 CO 2 RR 和 H 2的速率决定步骤的势垒进化因此在两个领域表现出出色的催化能力。这项工作展示了Cu 0和Cu 2+对提高CO 2 RR 和H 2释放的光热催化性能的协同作用,并提供了一种合成金属-半导体纳米结构的新策略,以有效地将太阳能转化为燃料。