空心分层 Cu2O 衍生电催化剂在低过电势下引导 CO2 还原为多碳化学品,Advanced Materials

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空心分层 Cu2O 衍生电催化剂在低过电势下引导 CO2 还原为多碳化学品
Advanced Materials ( IF 27.4 ) Pub Date : 2023-04-29 , DOI: 10.1002/adma.202301127
Jinhan Li ₁ , Keqiang Xu ₁ , Fangming Liu ₁ , Youzeng Li ₁ , Yanfang Hu ₁ , Xijie Chen ₁ , Huan Wang _{1,

2} , Wence Xu ₁ , Youxuan Ni ₁ , Guoyu Ding ₁ , Tete Zhao ₁ , Meng Yu _{1,

2} , Wei Xie ₁ , Fangyi Cheng _{1,

2}

Affiliation

利用可再生电力将二氧化碳电化学还原为多碳产品（C _{2+ ），为能源和环境可持续发展提供了一条有前途的途径。}已经展示了各种氧化物衍生的铜（OD-Cu）催化剂，但由于碳-碳键形成缓慢和CO中间体（*CO）覆盖率低，仍然需要高过电势来驱动C _2+生产。在这里，通过精心设计 OD-Cu 形貌来规避这个困境。首先，计算研究提出了一种中空且分层的OD-Cu微结构，该结构可以产生核壳微环境，抑制CO析出并通过中间限制和电场增强加速*CO二聚化，从而提高C ₂₊一代。实验上，设计的纳米结构是通过杂种诱导方法合成的，然后进行电化学活化。原位光谱研究进一步阐述了 *CO 二聚化与设计结构之间的相关性。_{值得注意的是，分级OD-Cu表现出CO 2}还原的形态依赖性选择性，与可逆氢电极相比，在-0.55 V的相当大的正电势下，C _{2+法拉第效率为75.6%。}

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Hollow Hierarchical Cu2O-Derived Electrocatalysts Steering CO2 Reduction to Multi-Carbon Chemicals at Low Overpotentials

The electrochemical reduction of carbon dioxide into multi-carbon products (C₂₊) using renewably generated electricity provides a promising pathway for energy and environmental sustainability. Various oxide-derived copper (OD-Cu) catalysts have been showcased, but still require high overpotential to drive C₂₊ production owing to sluggish carbon–carbon bond formation and low CO intermediate (*CO) coverage. Here, the dilemma is circumvented by elaborately devising the OD-Cu morphology. First, computational studies propose a hollow and hierarchical OD-Cu microstructure that can generate a core–shell microenvironment to inhibit CO evolution and accelerate *CO dimerization via intermediate confinement and electric field enhancement, thereby boosting C₂₊ generation. Experimentally, the designed nanoarchitectures are synthesized through a heteroseed-induced approach followed by electrochemical activation. In situ spectroscopic studies further elaborate correlation between *CO dimerization and designed architectures. Remarkably, the hierarchical OD-Cu manifests morphology-dependent selectivity of CO₂ reduction, giving a C₂₊ Faradaic efficiency of 75.6% at a considerably positive potential of −0.55 V versus reversible hydrogen electrode.

更新日期：2023-04-29

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