Transition Metal and Metal-N-x Codoped MOF-Derived Fenton-Like Catalysts: A Comparative Study on Single Atoms and Nanoparticles
Transition Metal and Metal-N-x Codoped MOF-Derived Fenton-Like Catalysts: A Comparative Study on Single Atoms and Nanoparticles
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过渡金属和金属-N-x共掺杂MOF衍生的类芬顿催化剂：单原子和纳米粒子的比较研究
DOI：
10.1002/smll.202005060
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发表时间：
2020
期刊：
影响因子：
13.3
通讯作者：
Cheng Chong
中科院分区：
文献类型：
--
作者：
Gao Yun;Yang Chengdong;Zhou Mi;He Chao;Cao Sujiao;Long Yanping;Li Shuang;Lin Yi;Zhu Puxin;Cheng Chong
为了处理水系统中不断增长的有毒苯衍生化合物，人们已经致力于催化降解污染物。然而，在类芬顿反应中，基于过渡金属的纳米颗粒或单原子位点的活性和效率仍然不明确。在本文中，为了比较纳米颗粒和单个原子的类芬顿催化效率，制造包含Co纳米晶体和Co-Nx共掺杂的碳纳米管（CNT）或裸Co-Nx掺杂的CNT的独立式纳米纤维催化剂。值得注意的是，所有这些纳米纤维催化剂表现出有效的活性，介孔结构和导电碳网络，这使得催化效果的可行性验证。得益于最大化的原子利用率，原子Co-Nx中心表现出更高的反应动力学常数（κ = 0.157 min−1）和对双酚A降解的质量活性，远远超过Co纳米晶体（κ = 0.082 min−1）。然而，对于体积活性，单原子催化剂与基于金属的催化剂相比没有显示出明显的优势。总体而言，这项工作不仅为比较基于过渡金属的纳米颗粒或单个原子的芬顿类催化效应提供了一条可行的途径，而且为开发用于有机污染物降解的突出催化剂开辟了一条新途径。
To deal with the ever‐growing toxic benzene‐derived compounds in the water system, extensive efforts have been dedicated for catalytic degradation of pollutants. However, the activities and efficiencies of the transition metal‐based nanoparticles or single‐atom sites are still ambiguous in Fenton‐like reactions. Herein, to compare the Fenton‐like catalytic efficiencies of the nanoparticles and single atoms, the free‐standing nanofibrous catalyst comprising Co nanocrystals and Co–Nxcodoped carbon nanotubes (CNTs) or bare Co–Nxdoped CNTs is fabricated. It is noteworthy that all these nanofibrous catalysts exhibit efficient activities, mesoporous structures, and conductive carbon networks, which allow a feasible validation of the catalytic effects. Benefiting from the maximized atomic utilization, the atomic Co–Nxcenters exhibit much higher reaction kinetic constant (κ = 0.157 min−1) and mass activity toward the degradation of bisphenol A, far exceeding the Co nanocrystals (κ = 0.082 min−1). However, for the volume activities, the single‐atom catalyst does not show apparent advantages compared to the nanocrystal‐based catalyst. Overall, this work not only provides a viable pathway for comparing Fenton‐like catalytic effects of transition metal‐based nanoparticles or single atoms but also opens up a new avenue for developing prominent catalysts for organic pollutants’ degradation.