<br>用于水相光电化学 CO2 还原生成甲酸盐和合成气的高效 Cu2O 光阴极,Journal of the American Chemical Society

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用于水相光电化学 CO2 还原生成甲酸盐和合成气的高效 Cu2O 光阴极
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-12-13 , DOI: 10.1021/jacs.3c06146
Meng Xia ₁ , Linfeng Pan ₁ , Yongpeng Liu ₂ , Jing Gao ₁ , Jun Li ₁ , Mounir Mensi ₃ , Kevin Sivula ₂ , Shaik M Zakeeruddin ₁ , Dan Ren _{1,

4} , Michael Grätzel ₁

Affiliation

光电化学二氧化碳还原（PEC–CO ₂ R）是利用太阳能生产可再生燃料和化学品的一种有前景的方法。然而，即使要获得适度的太阳能到燃料（STF）转换效率，通常也需要使用昂贵的半导体和贵金属催化剂。在此，我们通过简单的光电化学沉积方法提出了一种用Sn/SnO _x催化剂修饰的Cu ₂ O/Ga ₂ O ₃ /TiO ₂光阴极。在AM 1.5 G 光照下，KHCO ₃电解质水溶液中的CO ₂ R 半电池STF 效率达到约0.31%。该系统能够高效生产合成气（FE：∼62%，CO/H ₂ ≈ 1:2）和甲酸盐（FE：∼38%），并且在+0.34至-0.16 V vs 的宽电位范围内具有一致的选择性。可逆氢电极。我们将观察到的性能归因于我们的 Cu ₂ O 异质结构和 PEC-CO ₂ R 反应中采用的高效 Sn/SnO _x催化剂的有利光电特性。通过全面的实验研究，我们阐明了 Cu ₂ O 埋入式 p-n 结在产生高光电压（∼1 V）和实现有效的体电荷分离（高达 ∼70% 效率）方面不可或缺的作用。同时，我们发现沉积的Sn/SnO _x催化剂对PEC器件的整体性能具有关键的双重影响，既充当活性CO ₂ R催化剂又充当半导体前接触。它可以通过建立无障碍欧姆接触来促进催化剂和CO ₂ R半导体器件之间的界面电子转移。

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Efficient Cu2O Photocathodes for Aqueous Photoelectrochemical CO2 Reduction to Formate and Syngas

Photoelectrochemical carbon dioxide reduction (PEC–CO₂R) represents a promising approach for producing renewable fuels and chemicals using solar energy. However, attaining even modest solar-to-fuel (STF) conversion efficiency often necessitates the use of costly semiconductors and noble-metal catalysts. Herein, we present a Cu₂O/Ga₂O₃/TiO₂ photocathode modified with Sn/SnO_x catalysts through a simple photoelectrodeposition method. It achieves a remarkable half-cell STF efficiency of ∼0.31% for the CO₂R in aqueous KHCO₃ electrolyte, under AM 1.5 G illumination. The system enables efficient production of syngas (FE: ∼62%, CO/H₂ ≈ 1:2) and formate (FE: ∼38%) with a consistent selectivity over a wide potential range, from +0.34 to −0.16 V vs the reversible hydrogen electrode. We ascribe the observed performance to the favorable optoelectronic characteristics of our Cu₂O heterostructure and the efficient Sn/SnO_x catalysts incorporated in the PEC–CO₂R reactions. Through comprehensive experimental investigations, we elucidate the indispensable role of Cu₂O buried p–n junctions in generating a high photovoltage (∼1 V) and enabling efficient bulk charge separation (up to ∼70% efficiency). Meanwhile, we discover that the deposited Sn/SnO_x catalysts have critical dual effects on the overall performance of the PEC devices, serving as active CO₂R catalysts as well as the semiconductor front contact. It could facilitate interfacial electron transfer between the catalysts and the semiconductor device for CO₂R by establishing a barrier-free ohmic contact.

更新日期：2023-12-13

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