Mingxiang Zhang , Wen Luo , Shanghao Gu , Weihan Xu , Zhouguang Lu , Fei Wang
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引用次数: 0
摘要
光电化学(PEC)技术完美地整合并优化了光催化和电催化的优点,促进了电荷分离并提高了太阳能转换效率。它是一种很有前景的二氧化碳处理方法。氮化镓作为Ⅲ-Ⅴ族半导体,在 PEC CO2 还原反应 (RR) 领域受到了广泛关注。本研究通过直接水热合成法制备了 GaN 和 In/GaN 微棒。在-0.75 VRHE(可逆氢电极,RHE)条件下,In/GaN 的电流密度约为 10 mA/cm2,一氧化碳法拉第效率(FE)为 45%,在 2 小时的 PEC CO2 还原反应中表现出卓越的稳定性。在 GaN 中引入 In 能显著提高二氧化碳吸附能力和光收集能力。此外,密度泛函理论(DFT)计算阐明,掺杂 In 的 GaN 可以减少中间 CO 的吸附,有利于随后的 CO 解吸。此外,N-空位随着铟的掺入而增加,导致非配对电子的数量增加,从而促进了载流子的传输。在此,我们引入了振动能量收集器来驱动 CO2 RR,这标志着 PEC CO2 RR 在未来绿色能源应用领域的发展取得了重大进展。
Photoelectrochemical catalytic CO2 reduction enhanced by In-doped GaN and combined with vibration energy harvester driving CO2 reduction
Photoelectrochemical (PEC) technology seamlessly integrates and optimizes the merits of photocatalysis and electrocatalysis, facilitating charge separation and enhancing solar conversion efficiency. It stands out as a promising approach for CO2 treatment. GaN as III-Ⅴ semiconductor, has garnered substantial attention in the realm of PEC CO2 reduction reactions (RR). In this study, GaN and In/GaN micro-rods were prepared via straightforward hydrothermal synthesis. Attaining a current density of approximately 10 mA/cm2 and CO Faradaic Efficiency (FE) of ∼45 % at −0.75 VRHE (Reversible Hydrogen Electrode, RHE), In/GaN exhibited exceptional stability over a 2 h PEC CO2 RR. The introduction of In into GaN significantly augmented CO2 adsorption capacity and light harvesting. Additionally, Density Functional Theory (DFT) calculations elucidated that In-doped GaN can diminish the adsorption of intermediate CO, favoring subsequent CO desorption. Furthermore, the N-vacancy increased with In doping, resulting in a rise in the number of unpaired electrons, facilitating carrier transport. Herein, vibration energy harvester was introduced to drive CO2 RR, marking a significant advancement in development of PEC CO2 RR for future green energy applications.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.