Hydrogen spillover involves the dissociation of H₂ on transition metal nanoparticles and further atomic hydrogen surface migration on catalyst supports. Hence, the spillover phenomenon has been reported in applications of heterogeneous catalysis in hydrogenation and room-temperature hydrogen storage. However, a proper catalyst design is requisite to initiate hydrogen spillover, considering the transition metal particle dispersion, sorbent surface modification, porosity, etc. In this report, we pyrolyzed the zeolitic imidazolate framework ZIF-67 for residual Co metal nanoparticles and N-dopant on ZIF-derived carbon (ZDC) for hydrogen adsorption via spillover effect. Catalyst optimization by proper ZIF carbonization process regarding manipulated pyrolytic temperatures, atmospheres, and ramping rates, results in different properties in ZDCs. Well-distributed Co nanoparticles can be obtained on N-rich graphitic sorbent ZDCs with retained high specific surface area. The Co on ZDC exhibits improved room-temperature hydrogen capacity of 0.77 wt% than neat ZIF-67 of 0.09 wt% at 30 bar, 300 K. The adsorption sites were examined experimentally by nitrogen hydrogenation, and possible atomic hydrogen diffusion was evaluated theoretically showing energy barrier reduced by over 0.1 eV. It demonstrates that cobalt nanoparticles can successfully initiate hydrogen spillover on ZIF-derived carbon with nitrogen functionality, even without noble metals.

_{氢气溢出涉及 H 2}的解离过渡金属纳米粒子和催化剂载体上进一步原子氢表面迁移。因此，在多相催化加氢和室温储氢应用中已经报道了溢出现象。然而，考虑到过渡金属颗粒分散、吸附剂表面改性、孔隙率等，适当的催化剂设计对于引发氢溢出是必要的。在本报告中，我们热解沸石咪唑酯骨架ZIF-67，产生残留的Co金属纳米颗粒和ZIF衍生碳（ZDC）上的N掺杂剂，通过溢出效应吸附氢。通过适当的 ZIF 碳化过程对受控热解温度、气氛和升温速率进行催化剂优化，导致 ZDC 具有不同的特性。在富氮石墨吸附剂 ZDC 上可以获得分布良好的 Co 纳米粒子，并保留高比表面积。在 30 bar、300 K 条件下，ZDC 上的 Co 的室温氢容量比纯 ZIF-67 的 0.09 wt% 提高了 0.77 wt%。通过氮氢化实验检查了吸附位点，并从理论上评估了可能的原子氢扩散，显示能垒降低了 0.1 eV 以上。它表明，即使没有贵金属，钴纳米颗粒也可以成功地在具有氮功能的 ZIF 衍生碳上引发氢溢出。通过氮氢化对吸附位点进行了实验检查，并从理论上评估了可能的原子氢扩散，结果表明能垒降低了 0.1 eV 以上。它表明，即使没有贵金属，钴纳米颗粒也可以成功地在具有氮功能的 ZIF 衍生碳上引发氢溢出。通过氮氢化对吸附位点进行了实验检查，并从理论上评估了可能的原子氢扩散，结果表明能垒降低了 0.1 eV 以上。它表明，即使没有贵金属，钴纳米颗粒也可以成功地在具有氮功能的 ZIF 衍生碳上引发氢溢出。