摘要
Sulfur and nitrogen dual-doped graphdiyne(NSGD)has been found to be a promising catalyst for oxygen reduction reaction(ORR)through a combination of density functional theory(DFT)calculation and the application of oxygen evolution reaction(OER)experiments.The DFT analysis suggests that adsorption characteristics are significantly altered by resulting nitrogen and sulfur doping,which in turn affect the ORR activity.In particular,the NSGD-800 catalyst exhibits an increased ORR half-wave potential of 0.754 V,with enhanced stability due to the synergy effect of N and S.Meanwhile,thanks to the unique acetylene-rich structure of graphdiyne to anchor metal oxides with strong d-πinteractions,the activity and stability of com-RuO2 for OER were significantly enhanced by mixing with NSGD-800.The zinc-air battery(ZAB)with NSGD shows a much higher peak power density(87.3 mW cm^(−2))and longer charge-discharge cycle stability compared with the ZAB with Pt/C,making it an excellent candidate air electrode for ZAB and other energy storage and conversion devices.
通过密度泛函理论(DFT)计算与实验相结合的方法,硫氮双掺杂石墨炔(NSGD)是一种极具潜力的氧还原反应(ORR)和氧析出反应(OER)助催化剂.DFT揭示了氮和硫的掺杂显著改变了材料的吸附特性,从而显著提升了ORR活性.其中,NSGD-800催化剂的ORR半波电位高达0.754 V,表现出优异的催化性能.同时,当NSGD-800与商业RuO2机械混合后的OER活性和稳定性得到显著增强.研究结果表明,石墨炔(GDY)独特的富乙炔结构使其成为锚定金属的理想载体,而具有强d-π相互作用的氧化物可进一步提高OER的活性和稳定性.由上述制备的硫氮双掺杂石墨炔基ORR与OER催化剂组装的锌空电池(ZAB)展现出卓越的性能,其最大功率密度达到87.3 mW cm^(−2)并且具有更长的充放电循环稳定性.这些优异特性使NSGD成为ZAB及其他储能转换装置空气电极的理想选择.
基金
supported by the National Natural Science Foundation of China(22202037 and 22102105)
the Fundamental Research Funds for the Central Universities(2412023QD019 and 2412024QD014)
the support from grants under the Science and Technology Development Plan Project of Jilin Province,China(20240101192JC)
seventh batch of the Jilin Province Youth Science and Technology Talent Lifting Project(QT202305)。
