Lulu Li, Bing Nan, Neng Neng Xu, Ge Bai, Ruinan He, Yuyu Liu, Jinli Qiao
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引用次数: 0
摘要
在光电催化一氧化碳还原(PEC CO)反应中,开发合适的光电阴极以实现高光电流和长期耐久性仍然是一个巨大的挑战。本文通过自组装工艺设计了一种掺杂 In 的生物氧化物装饰氧化泡沫铜(CBIO/CF)自立光电阴极,无需外部添加粘合剂。通过太阳光促进策略,具有独特三维分层纳米花结构的 CBIO/CF 在 -0.87 ∼ -1.17 V 的宽电位窗口内对 HCOOH 显示出 90.0 % 的卓越远电效率,在 -0.87 V 时达到 97.8 %,部分电流密度为 14.41 mA cm。原位傅立叶变换红外光谱(FTIR)分析表明,掺杂 In 引发的大量氧缺陷促进了 CBIO/CF 吸收与甲酸盐生成有关的实质性中间物种,而多孔结构则加速了质量传输。此外,催化剂表面精心设计的 CuO 和 In 掺杂的 BiO 交错 p-n 异质结有利于电子/空穴对的产生和分离,有助于在偏置电压下光催化还原 CO。这项工作为合理调节 PEC CO 到 HCOOH 的自支撑光电极,使其具有合适的导带价带、高性能和高稳定性铺平了道路。
Sunlight-promoted CO2 electroreduction with staggered p-n heterojunction by indium-doped bismuth 3D nanoflower structure on oxidized copper foam as self-standing photoelectric cathode over a wide potential window
Exploiting suitable photocathodes to achieve high photocurrent and long-term endurance is still a great challenge in photoelectrocatalytic CO reduction (PEC CO) reactions. Herein, an In-doped BiO decorated oxidized copper foam (CBIO/CF) self-standing photoelectric cathode is well designed by the self-assembly process without an externally added binder. Via sunlight-promoted strategy, CBIO/CF with a unique 3D hierarchical nanoflower structure displays a superior faradaic efficiency of 90.0 % towards HCOOH over a wide potential window from −0.87 ∼ −1.17 V and reaches 97.8 % at −0.87 V with a partial current density of 14.41 mA cm. The in-situ Fourier transform infrared spectroscopy (FTIR) analysis demonstrates the abundant oxygen defects induced by In doping boost CBIO/CF absorbing substantive intermediate species related with formate generations, and porous structure accelerating mass transportation. Moreover, the well-designed staggered p-n heterojunctions of CuO and In-doped BiO on the surface of catalysts favor the generation and separation of electron/hole pairs and contribute to the photocatalytic reduction of CO under a bias voltage. This work paves the way for rational regulation of self-supporting photoelectrode for PEC CO to HCOOH with suitable conduction band valence bands and high performance and stability.