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Regulating the Product Distribution of CO Reduction by the Atomic-Level Structural Modification of the Cu Electrode Surface

机译：通过铜电极表面的原子级结构修饰来调节CO还原产物的分布

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摘要

Cu catalyzes the electrochemical reduction of CO2 or CO to an assortment of products, a behavior that is a detriment when only one reduced compound is desired. The present article provides an example in which, through the atomic-level control of the structure of the Cu electrode surface, the yield distribution is regulated to generate only one product. The reaction investigated was the preferential reduction of CO to C2H5OH on Cu at a low overpotential in alkaline solution. Experimental measurements combined electrochemical scanning tunneling microscopy (ECSTM) and differential electrochemical mass spectrometry (DEMS). An atomically ordered Cu(100) surface, prepared from either a single crystal or by Cu(pc)-to-Cu(100) reconstruction, did not produce ethanol. When the surfaces were subjected to monolayer-limited Cua dagger"Cu2O cycles, only the reconstructed surface underwent an additional structural transformation that spawned the selective production of ethanol at a potential 645 mV lower than that which generates multiple products. Quasi-operando ECSTM indicated transformation to an ordered stepped surface, Cu(S) -aEuroe[3(100) x (111)], or Cu(511). The non-selective, multiple-product Cu-catalyzed reduction of CO had thus been regulated to yield only one liquid fuel by an atomic-level structural modification of the electrode surface.
机译：Cu催化将CO 2或CO的电化学还原成多种产物，当仅需要一种还原的化合物时，这种行为是有害的。本文提供了一个示例，其中，通过原子级控制Cu电极表面的结构，调节了屈服分布以仅生成一种产物。研究的反应是在碱性溶液中以低过电势将CO在Cu上优先还原为C2H5OH。实验测量结合了电化学扫描隧道显微镜（ECSTM）和差分电化学质谱（DEMS）。由单晶或通过Cu（pc）-to-Cu（100）重建制备的原子有序的Cu（100）表面不会产生乙醇。当对表面进行单层限制的Cua匕首“ Cu2O”循环时，仅重构的表面经历了额外的结构转变，从而产生了比产生多种产物的电势低645 mV的乙醇选择性生产。准操作数ECSTM指示了转变到有序台阶表面Cu（S）-aEuroe [3（100）x（111）]或Cu（511），因此非选择性的多产物Cu催化的CO还原反应已被调节为仅产生一种液体燃料，是通过对电极表面进行原子级的结构改性而制成的。

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