Singla Gourav, Bhange Siddheshwar N, Mahajan Mani, Kurungot Sreekumar
Physical and Materials Chemistry Division, CSIR-National Chemical Laboratory, Pune, Maharashtra 411008, India.
Nanoscale. 2021 Mar 28;13(12):6248-6258. doi: 10.1039/d0nr09156a. Epub 2021 Mar 22.
In this work, a strategy has been adopted to construct an architecture through the coordination of polyvinylpyrrolidone (PVP) and a monodisperse zeolitic imidazolate framework (ZIF-8), which was entwined by carbon nanotubes (CNTs) firstly, followed by a pyrolysis process to obtain the hybrid catalyst. The meticulous design of the hybrid material using CNTs to interconnect the PVP assisted ZIF-8 derived porous carbon frameworks together produces a hierarchical pore structure and dual-heteroatom (Zn/N) doping (Zn-N/PC@CNT). Without further acid treatment, the hybrid material prepared after pyrolysis at 900 °C (PVP-ZIF-8@CNT-900) has been demonstrated as an efficient non-precious metal catalyst for the oxygen reduction reaction (ORR) with its superior stability compared to the commercial 20 wt% Pt/C catalyst in alkaline media. The catalyst shows better performance towards the ORR, with its more positive onset and half-wave potentials (E = 0.960 V vs. RHE and E = 0.795 V vs. RHE) than the counterpart system which is free of both CNT and PVP. The high performance of the hybrid catalyst can be ascribed to the co-existence of dual-active sites with hierarchical pore structures originating from the synergistic effects between Zn/N co-doped porous carbon and CNTs. We further demonstrated the single-cell performance by using the homemade system as the cathode catalyst for the Alkaline Exchange Membrane Fuel Cell (AEMFC) system, which showed a maximum power density of 45 mW cm compared to 60 mW cm obtained from the 40 wt% Pt/C catalyst.
在这项工作中,采用了一种策略,通过聚乙烯吡咯烷酮(PVP)与单分散沸石咪唑酯骨架(ZIF-8)的配位来构建一种结构,首先将ZIF-8与碳纳米管(CNT)缠绕,然后经过热解过程以获得混合催化剂。使用CNT将PVP辅助的ZIF-8衍生的多孔碳骨架相互连接在一起,对混合材料进行精心设计,产生了分级孔结构和双杂原子(Zn/N)掺杂(Zn-N/PC@CNT)。无需进一步酸处理,在900℃热解后制备的混合材料(PVP-ZIF-8@CNT-900)已被证明是一种用于氧还原反应(ORR)的高效非贵金属催化剂,在碱性介质中与商业20 wt% Pt/C催化剂相比具有优异的稳定性。该催化剂对ORR表现出更好的性能,其起始电位和半波电位(相对于可逆氢电极,E = 0.960 V和E = 0.795 V)比不含CNT和PVP的对应体系更正。混合催化剂的高性能可归因于双活性位点与分级孔结构的共存,这源于Zn/N共掺杂多孔碳与CNT之间的协同效应。我们进一步通过使用自制系统作为碱性交换膜燃料电池(AEMFC)系统的阴极催化剂来展示单电池性能,该系统显示出最大功率密度为45 mW/cm²,而40 wt% Pt/C催化剂获得的最大功率密度为60 mW/cm²。