Browsing by Author "Shen, Huidong"

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    Achieving Highly Selective Electrocatalytic CO2 Reduction by Tuning CuO-Sb2O3 Nanocomposites
    (ACS Sustainable Chemistry & Engineering, 2020) Li, Yangmei; Chu, Senlin; Shen, Huidong; Xia, Qineng; Robertson, Alex W.; Masa, Justus; Siddiqui, Umer; Sun, Zhenyu
    The development of highly active and selective electrocatalysts with low cost and earth abundance for electrochemical CO2 reduction (ECR) remains an important area of interest. Here, we report the modification of CuO with other metal (Bi, Sb, Cd, and Zr) oxides to form bimetallic oxide nanocomposite catalysts exhibiting efficient ECR. In particular, CuO-Sb2O3 nanoparticles anchored on carbon black (CB) facilitated ECR selectively to CO at low overpotentials, providing a CO faradaic efficiency (FE) of up to 90.0% at −0.8 V versus reversible hydrogen electrode, in contrast to individual CuO/CB and Sb2O3/CB, which gave rise to CO FEs of less than 31.0%, outperforming many previously reported catalysts. A strong interaction between CuO and Sb2O3 is found, which likely contributes to the enhanced ECR activity.
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    Electrochemical Ammonia Synthesis: Mechanistic Understanding and Catalyst Design
    (Chem,, 2021) Shen, Huidong; Choi, Changhyeok; Masa, Justus; Qiu, Jieshan; Jung, Yousung; Sun, Zhenyu
    NH3 production is dependent on the century-old Haber-Bosch process, which is energy and capital intensive and relies on H2 from steam reforming, hence, contributing to greenhouse gas emissions. Electrochemical NH3 synthesis can be realized by reaction of N2 and a proton source under mild conditions powered by renewable electricity, which offers a promising carbon-neutral and sustainable strategy. However, N2 has remarkable thermodynamic stability and requires high energy to be activated. Implementation of this “clean” NH3 synthesis route therefore still requires significant enhancement in energy efficiency, conversion rate, and durability, which is only achievable through the design of efficient electrocatalysts. This article provides a timely theoretical and experimental overview of recent advances in the electrocatalytic conversion of N2 to NH3 underlining the development of novel electrocatalysts. Advances of in situ and operando studies for mechanistic understanding of the reaction and the main challenges and strategies for improving electrocatalytic N2 reduction are highlighted.