在具有暴露晶界的亚2纳米SnO量子线上将CO高效电化学还原为HCOOH
Efficient Electrochemical Reduction of CO to HCOOH over Sub-2 nm SnO Quantum Wires with Exposed Grain Boundaries.
作者信息
Liu Subiao, Xiao Jing, Lu Xue Feng, Wang Jiong, Wang Xin, Lou Xiong Wen David
机构信息
School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore.
Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, T6G 1H7, Canada.
出版信息
Angew Chem Int Ed Engl. 2019 Jun 17;58(25):8499-8503. doi: 10.1002/anie.201903613. Epub 2019 May 17.
Electrochemical reduction of CO could mitigate environmental problems originating from CO emission. Although grain boundaries (GBs) have been tailored to tune binding energies of reaction intermediates and consequently accelerate the CO reduction reaction (CO RR), it is challenging to exclusively clarify the correlation between GBs and enhanced reactivity in nanostructured materials with small dimension (<10 nm). Now, sub-2 nm SnO quantum wires (QWs) composed of individual quantum dots (QDs) and numerous GBs on the surface were synthesized and examined for CO RR toward HCOOH formation. In contrast to SnO nanoparticles (NPs) with a larger electrochemically active surface area (ECSA), the ultrathin SnO QWs with exposed GBs show enhanced current density (j), an improved Faradaic efficiency (FE) of over 80 % for HCOOH and ca. 90 % for C1 products as well as energy efficiency (EE) of over 50 % in a wide potential window; maximum values of FE (87.3 %) and EE (52.7 %) are achieved.
电化学还原CO可以减轻因CO排放而产生的环境问题。尽管人们已经对晶界（GBs）进行了调控，以调节反应中间体的结合能，从而加速CO还原反应（CO RR），但要专门阐明GBs与小尺寸（<10 nm）纳米结构材料中增强的反应活性之间的相关性仍具有挑战性。现在，合成了由单个量子点（QDs）和表面大量GBs组成的亚2 nm SnO量子线（QWs），并研究了其在CO RR生成HCOOH方面的性能。与具有较大电化学活性表面积（ECSA）的SnO纳米颗粒（NPs）相比，具有暴露GBs的超薄SnO QWs在较宽的电位窗口中显示出增强的电流密度（j）、超过80%的HCOOH和约90%的C1产物的改进法拉第效率（FE）以及超过50%的能量效率（EE）；实现了FE（87.3%）和EE（52.7%）的最大值。
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