硼氮双掺杂提升碳点电催化氧还原活性研究

摘要

碳点(CDs)因其较大的比表面积和较快的电子转移特性,已成为能量转换应用领域一种新兴的纳米炭材料。本文以低成本的石油焦为原料,通过简便的一步电化学刻蚀方法制备了硼氮双掺杂碳点(BN-CDs)。与单掺杂碳点B-CDs和N-CDs相比,双掺杂BN-CDs表现出更优异的四电子氧还原电催化活性,具有更正的起始电位(Eonset=0.958 V)和大的扩散极限电流密度(j D=-4.32 mA cm~(-2)),且长期稳定性和甲醇耐受性优于商用Pt/C催化剂。密度泛函理论计算(DFT)研究表明,B、N双掺杂的协同效应促进了O_2分子的吸附,有助于提高碳点的电催化活性。本研究为纳米炭材料的设计及其在能量转换领域的应用提供了新的思路。Carbon dots(CDs)have become an emerging carbon nanomaterial for use in energy-conversion systems because of their large surface area and rapid electron transfer.Carbon dots(BN-CDs)doped with both boron and nitrogen were synthesized by a simple one-step electrochemical etching approach using low-cost petroleum coke as precursor.Compared with CDs doped with only B or N,BN-CDs showed an excellent four-electron oxygen reduction reaction(ORR)activity with a positive onset potential of 0.958 V and a large diffusion-limited current density of-4.32 mA cm-2.Furthermore,the long-term stability and methanol tolerance of BN-CDs were better than those of a commercial Pt/C catalyst.It was found by density functional theory(DFT)calculation that the co-doping of N and B promoted the adsorption of O2 molecules in the ORR process.This work provides new insight into the rational design of carbon nanomaterials and their use in energy conversion.

作者刘卉刘子慧张金强智林杰吴明铂LIU Hui;LIU Zi-hui;ZHANG Jin-qiang;ZHI Lin-jie;WU Ming-bo(State Key Laboratory of Heavy Oil Processing,College of New Energy,College of Chemical Engineering,China University of Petroleum(East China),Qingdao 266580,China;School of Engineering,Edith Cowan University,270 Joondalup Drive,Joondalup,WA 6027,Australia;College of New Energy,China University of Petroleum(East China),Qingdao 266580,China)

机构地区中国石油大学（华东）新能源学院 School of Engineering 中国石油大学（华东）新能源学院

出处《新型炭材料》 SCIE EI CAS CSCD 北大核心 2021年第3期585-593,共9页New Carbon Materials

基金国家自然科学基金(52072409,U1662113,U20A20131) 山东省泰山学者人才工程项目(ts201712020).

关键词碳点硼掺杂氮掺杂氧还原Carbon dots Boron doping Nitrogen doping Oxygen reduction reaction

分类号TB33 [一般工业技术—材料科学与工程]

相关文献