近日，我院唐东升教授课题组在Science China Materials发表题为“Maximizing hydrogn evolution via Co-Ni dual atoms and nanoclusters on hierarchically ordered porous carbon framework”的学术论文。

该团队使用多金属单晶有序大孔金属-有机框架（MOFs）作为前体，合成了CoNi SAs@NPs-NC催化剂。该催化剂具有大孔和微孔的多级孔结构，该结构不仅提供了高比表面积，还提供了快速的物质扩散通道。此外，该催化剂具有的双金属组分，以及单原子（SAs）和纳米颗粒（NPs）之间的协同作用显著增强了其催化活性。CoNi SAs@NPs-NC纳米催化剂在析氢反应中展示了卓越的活性, 在1 M的KOH和0.5 M的H₂SO₄中分别具有90和61 mV的过电势（电流密度10 mA cm⁻²）。本研究还使用密度泛函理论（DFT）分析了CoNi NPs与SAs之间的协同作用。本工作展示了CoNi SAs@NPs-NC催化剂在高效析氢中的潜力。

唐东升教授为该论文的第一通讯作者，李谦讲师为论文的第一作者，湖南师范大学为第一单位。北京大学张盼博士、国家纳米科学中心李群博士和清华大学吴佳宾博士为论文的共同通讯作者。该工作获得了国家自然科学基金、湖南省教育厅自然科学基金等资助。

Figure 1. Synthesis and characterization of SOM ZnCoNi-ZIFs. (a) The schematic diagram of the process for the preparation of SOM ZnCoNi-ZIFs and its derivative CoNi SAs@NPs-NC. (b) SEM image of ZnCoNi SOM-ZIFs. (c) N₂ adsorption-desorption isotherms. (d) Pore size distributions calculated by BJH model of SOM ZnCoNi-ZIFs and ZIF-8.

Figure 2. (a) TEM of CoNi SAs@NPs-NC. (b) High angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) image of CoNi SAs@NPs-NC. (c) AC STEM image of CoNi SAs@NPs-NC. (d) Corresponding EDX element mappings of the CoNi SAs@NPs-NC from (b). (e) TEM of CoNi SAs-NC. (f) HAADF-STEM image of CoNi SAs-NC. (g) AC STEM image of CoNi SAs-NC. (h) Corresponding EDX element mappings of the CoNi SAs-NC from (f). (i) TEM of Co SAs@NPs-NC. (j) HAADF-STEM image of Co SAs@NPs-NC. (k) AC STEM image of Co SAs@NPs-NC. (l) Corresponding EDX element mappings of the Co SAs@NPs-NC from (j).

Figure 3. HER performance of CoNi SAs@NPs-NC, Co SAs@NPs-NC and CoNi SAs-NC. (a) HER polarization curves in 1 M KOH. (b) HER polarization curves in 0.5 M H₂SO₄. (c) Chronoamperometry curve for 450,000 s in 0.1 V potential of CoNi SAs@NPs-NC. (d) Tafel slopes in 1 M KOH. (e) Tafel slopes in 0.5 M H₂SO₄. (f) Comparison of Tafel slopes and overpotentials at a current density of 10 mA cm⁻² of CoNi SAs@NPs-NC and the reported Co/Ni based catalysts (in 1 M KOH).

Figure 4. (a) Optimized structures of CoNi SAs-NC, Co SAs@NPs-NC and CoNi SAs@NPs-NC (Color scheme: C, brown; Co, blue; Ni, gray; N, white). (b) Free energies of the HER process in 0.5 M H₂SO₄.

论文链接：https://link.springer.com/article/10.1007/s40843-024-3012-4