Abstract The electrochemical reduction of CO2 (CO2RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials (SZ-HCN) as CO2RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area (1510 m2 g−g1) exhibited efficient electrocatalytic activity and selectivity for CO2RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency (~93%) at −0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2RR activity.

中文翻译：

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氮硫双掺杂高表面积空心碳纳米球可有效减少二氧化碳

摘要 CO2 电化学还原 (CO2RR) 可以极大地促进有用化学品的生产和减少全球 CO2 排放。在此，我们提出了作为 CO2RR 催化剂的 N 和 S 双掺杂高表面积碳材料（SZ-HCN）。N和S通过含N聚合物和S粉末的一步热解来掺杂。ZnCl2 用作挥发性致孔剂以制备多孔 SZ-HCN。具有高比表面积 (1510 m2 g-g1) 的 SZ-HCN 表现出高效的电催化活性和对 CO2RR 的选择性。电化学测量表明，SZ-HCN 在 -0.6 V 时具有高 CO 法拉第效率（~93%），显示出优异的 CO2-CO 还原催化性能。此外，SZ-HCN 提供稳定的电流密度和高 CO 选择性。至少 20 小时连续运行，显示出显着的电催化耐久性。实验结果和密度泛函理论计算表明，与单氮掺杂碳相比，N 和 S 双掺杂碳材料形成 COOH* 中间体所需的吉布斯自由能更低，从而提高了 CO2RR 活性.