Xiaowu Gao , Nan Li , Peize Li , Yan Wei , Qikang Huang , Kalsoom Akhtar , Esraa M. Bakhsh , Sher Bahadar Khan , Yan Shen , Mingkui Wang
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引用次数: 0
摘要
光电化学(PEC)还原二氧化碳是一种将二氧化碳转化为化学燃料以缓解环境危机的可行策略。然而,由于二氧化碳还原的光电催化动力学过程十分复杂,因此如何调控光电催化过程以获得理想的性能仍然是一项挑战。在此,我们提出了 ZnTe/SnS2 II 型异质结光催化剂,与纯 ZnTe 电极相比,该催化剂可促进光吸收,通过 PEC 还原 CO2 生成 CO,并具有更高的选择性和光稳定性。利用密度泛函理论(DFT)计算和扫描电化学显微镜(SECM)表征对 ZnTe/SnS2 异质结界面的电荷转移进行的研究表明,ZnTe 光产生的电荷可快速流经 ZnTe/SnS2 界面,在 II 型异质结内置电动势的驱动下参与 CO2 还原反应。在二氧化碳饱和的乙腈六氟磷酸四丁基铵电解液中,ZnTe/SnS2 光阴极在-1.78 V(相对于 Fc+/Fc)的标准光照条件下实现了 2.35 mA∙cm-2 的光电流密度和 87% 的二氧化碳远化效率,并且在连续光照测试一小时后仍能保持约 87% 的初始光电流。因此,在该电极上可获得 56.0 μM∙cm-2∙h-1 的 CO 生成率。
ZnTe/SnS2 heterojunction for photo-electrocatalysis of CO2 to CO
Photoelectrochemical (PEC) reduction of CO2 is a promising strategy to convert CO2 into chemical fuels for alleviating environmental crisis. However, modulation of photo-electrocatalytic processes to obtain a desired performance remains challenges due to the complicated PEC kinetics for CO2 reduction. Herein, we present ZnTe/SnS2 type II heterojunction photo-catalyst that facilitates light absorption for PEC reduction of CO2 toward CO production with an improved selectivity and photo-stability compared to the pure ZnTe electrode. The study of charge transfer at the ZnTe/SnS2 heterojunction interface with density functional theory (DFT) calculation and scanning electrochemical microscopy (SECM) characterization reveals that the photo-generated charge by ZnTe can flow quickly through the ZnTe/SnS2 interface to participate CO2 reduction reaction driven by the built-in electric potential of the type II heterojunction. The ZnTe/SnS2 photocathode achieves a photocurrent density of 2.35 mA∙cm−2 and a CO faradic efficiency of 87 % at −1.78 V (vs. Fc+/Fc) under standard illumination in a CO2-saturated tetrabutylammonium hexafluorophosphate in acetonitrile electrolyte, and retains approximately 87 % of its initial photocurrent after one-hour of continuous illumination test. Consequently, a generation rate of 56.0 μM∙cm−2∙h−1 for CO can be obtained on this electrode.
期刊介绍:
Electrochimica Acta is an international journal. It is intended for the publication of both original work and reviews in the field of electrochemistry. Electrochemistry should be interpreted to mean any of the research fields covered by the Divisions of the International Society of Electrochemistry listed below, as well as emerging scientific domains covered by ISE New Topics Committee.