多碳生成工厂: 用于提高CO2电催化生产率的CuO/Ni单原子串联催化剂
电化学CO2还原反应(CO2RR)的串联电催化策略是将CO2到C2+的多个步骤解耦为单独催化的CO2到CO和CO到C2+的两个步骤，以提高法拉第效率(FE)。然而，由于CO从生成位点到反应位点的传质限制，这种策略对于C2+的高速率生产仍然是挑战。
深圳大学苏陈良教授和中国科学技术大学吴宇恩教授课题组合作，设计合成了CuO/Ni单原子(SAs)串联催化剂，使得用于独立催化CO2-到-CO和CO-到-C2+的Ni和Cu的催化位点紧密相邻，能够原位产生和快速消耗CO。CuO/Ni SAs串联催化剂实现了高C2+的部分电流密度(1220.8 mA/cm2)，同时仍然保持了优异的C2+ FE(81.4%)。
Fig. 1. Synthesis and characterization of CuO/Ni SAs tandem catalyst. (a) Schematics of the synthesis (upper) and working (lower) mechanisms for CuO/Ni SAs tandem catalyst; (b) HAADF-STEM image of Ni SAs/N-C; (c, d) TEM and SEM images of CuO/Ni SAs (upper-right inset in Fig. 1c: HRTEM image of CuO/Ni SAs); (e) XPS of CuO/Ni SAs and CuO/N-C; (f) XRD patterns of CuO/Ni SAs, CuO/N-C, Ni SAs/N-C, and N-C; (g) EDS mapping of CuO/Ni SAs.
Fig. 2. The CO2RR performance comparisons of CuO/Ni SAs tandem catalyst composed by different mass ratios of CuO and Ni SAs/N-C. The C2+ products (a), C2H4 (b), and C2H5OH (c) FE comparisons for tandem catalysts of CuO/Ni SAs2.86, CuO/Ni SAs1.82, and CuO/Ni SAs1.27. The FE and products distribution for CuO/Ni SAs1.82 (d) and CuO/N-C (e). (f) The comparison for tandem catalysts CuO/Ni SAs2.86, CuO/Ni SAs1.82, CuO/Ni SAs1.27, and CuO/N-C. (g) The enhancement factors of C2+ products, C2H4, and C2H5OH FE for CuO/Ni SAs1.82 compared to CuO/N-C. (h) The stability of the tandem catalyst CuO/Ni SAs1.82. (i) The comparison of C2+ products FE for this work and previous reports [12, 17, 21, 22, 26, 27, 35-42], and the detailed data are shown in Table S1 (online).
Fig. 3. The comparisons of tandem catalyst electrodes fabricated with three strategies. The working mechanism schematics for tandem catalyst electrodes fabricated with strategies of physical mixing (a), layer-by-layer spraying (b), and adjacent nanostructure (c). The comparisons of tandem catalyst electrodes fabricated with three strategies in C2+ product FE (d), H2 FE (e), CO FE (f), and partial current densities of C2+ products (g).
Fig. 4. CO2RR performance of CuO/Ni SAs tandem catalyst in a MEA-based electrolyzer. (a) Cell structure of the MEA-based electrolyzer. The CO2RR performance (b) and stability (c) of the MEA cell equipped with CuO/Ni SAs tandem catalyst.
原 文 信 息
Yu Zhang, Peng Li , Changming Zhao, Fangyao Zhou, Qitao Zhang, Chenliang Su*, Yuen Wu*. Multicarbons generation factory: CuO/Ni single atoms tandem catalyst for boosting the productivity of CO2 electrocatalysis. Science Bulletin, 2022, 67(16):1679-1687