Abstract The search on low-cost, ultra-stable, and high-performance non-novel metal replacements to the Pt-based catalysts for oxygen reduction reaction (ORR) is of great urgency. Herein, a bottom-up method has been proposed to synthesize unique hollow N-doped carbon spheres (HNCSs) from an initial amorphous coordination polymer (CP) template-assisted route for the first time. HNCSs exhibit competitively comparable high electrocatalytic ORR activity, excellent reaction selectivity, and stronger long-term stability and negligible methanol crossover effect compared to the commercial Pt/C under the alkaline medium. Together with the other two reported carbonaceous ORR catalysts, including SCSs and NGPCs, our HNCSs possess the lowest Tafel slope of 65.7 mV dec−1 which is close to Pt/C (62.6 mV dec−1), and show much enhanced ORR activity (JL = 5.34 mA cm−2) and stability (Retention = 96.5%, Time = 10 h). This CP-templated route for hollow carbon materials will shed light on a new synthetic strategy to prepare high-performance carbon-based and/or metal-free ORR catalysts.

中文翻译：

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自下而上合成 MOF 衍生的空心 N 掺杂碳材料以提高 ORR 性能

摘要 寻找低成本、超稳定、高性能的非新型金属替代铂基氧还原反应（ORR）催化剂迫在眉睫。在此，首次提出了一种自下而上的方法，以从初始无定形配位聚合物 (CP) 模板辅助路线合成独特的空心 N 掺杂碳球 (HNCS)。在碱性介质下，与商业 Pt/C 相比，HNCS 表现出具有竞争力的高电催化 ORR 活性、优异的反应选择性、更强的长期稳定性和可忽略不计的甲醇交叉效应。连同其他两种报道的碳质 ORR 催化剂，包括 SCS 和 NGPC，我们的 HNCS 具有最低的 Tafel 斜率 65.7 mV dec-1，接近 Pt/C（62.6 mV dec-1），并显示出大大增强的 ORR 活性（ JL = 5。34 mA cm−2) 和稳定性（保留率 = 96.5%，时间 = 10 小时）。这种以 CP 为模板的中空碳材料路线将为制备高性能碳基和/或无金属 ORR 催化剂提供一种新的合成策略。