近日,实验室陈冰同学,周民杰在碳基材料的缺陷和形貌工程方面取得了巨大突破,为提高电化学能量转化和存储性能开辟了新的道路。该研究首次采用甲基橙和氯化铁组成的胶束对预合成的聚苯胺纳米管进行热解,成功制备了氮/硫共掺杂碳纳米管(NS-CNTs)。进一步,通过氨蚀刻引入固有碳缺陷和介孔,制得经氨蚀刻的NS-CNTs(ENSCNTs)复合材料。这种ENSCNTs材料充分结合了内在碳缺陷、外在N/S掺杂剂和多孔纳米管形态特征,极大地促进了其在氧还原反应(ORR)和硫还原反应(SRR)中的性能。这项研究为多功能碳基催化剂的缺陷和形态工程提供了新的策略,为电化学能量转换和存储领域的发展带来了希望。
Defects and morphology engineering is a serviceable strategy to boost the electrochemical energy conversion and storage performance of carbon-based materials. In this study, nitrogen/sulfur codoped carbon nanotubes (NS-CNTs) were first obtained via the pyrolysis of presynthesized polyaniline nanotubes with micelles composed of methyl orange and ferric chloride acting as the soft template. Furthermore, intrinsic carbon defects and mesopores were introduced to obtain etched NS-CNTs (ENS-CNTs) composites by ammonia etching. The rational combination of intrinsic/extrinsic defects and porous nanotube morphology features is beneficial to the oxygen reduction reaction (ORR) and sulfur reduction reaction (SRR) performances of the ENS-CNTs electrode. The coexistence of intrinsic carbon defects and extrinsic N/S dopants can create massive catalytically active sites for electrochemical processes, while the porous one-dimensional nanotube-like carbon framework is responsible for accessibility of catalytic active sites, species hosting, electrical conductivity, mass transport, and stability. Consequently, the ENS-CNTs-30 (where 30 represents the corresponding etching time in minutes) electrode for ORR displayed a high half-wave potential of 859 mV vs RHE, a diffusion limiting current density of 6.65 mA cm−2 , admirable stability, and methanol tolerance. The solid Zn−air battery (ZAB) assembled with ENS-CNTs-30 as the active material for the air cathode revealed remarkable power density (137 mW cm−2 ) and specific capacity (1467.4 mAh g−1 Zn). Meanwhile, the ENS-CNTs-30 electrode for SRR also demonstrated ameliorative
lithium−polysulfide (LiPS) trapping capability and Li2S deposition kinetics. The lithium−sulfur battery (LSB) with ENS-CNTs-30 as sulfur host material unfolded initial capacities of 1100 and 883 mAh g−1 at 0.2 and 2 C, respectively, and a capacity retention ratio of 82.0% after 200 cycles at 0.2 C. This work provides a feasible strategy for defects and morphology engineering of multifunctionalcarbon-based catalysts in electrochemical energy conversion and storage fields.
论文题目:Intrinsic Carbon Defects in Nitrogen and Sulfur Doped Porous Carbon Nanotubes Accelerate Oxygen Reduction and Sulfur Reduction for Electrochemical Energy Conversion and Storage.
论文作者:Minjie Zhou , Bing Chen , Na Zhang , Xianglin Deng , Xiating Jia , Jie Yang , HaiHua Yang.