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Boosting faradaic efficiency of CO_(2)electroreduction to CO for Fe-NC single-site catalysts by stabilizing Fe^(3+)sites via F-doping

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Nano Research 2022年第9期15卷 7896-7902页

作者： Yiqun Chen Guochang Li Yu Zeng Lijie Yan Xizhang Wang Lijun Yang Qiang Wu Zheng Hu Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Lab for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

The atomically dispersed Fe^(3+)sites of Fe-N-C single-site catalysts(SSCs)are demonstrated as the active sites for CO_(2)electroreduction(CO_(2)RR)to CO but suffer from the reduction to Fe^(2+)at~−0.5 V,accompanied by the drop of CO faradaic efficiency(FECO)and deterioration of partial current(JCO).Herein,we report the construction of F-doped Fe-N-C SSCs and the electron-withdrawing character of fluorine could stabilize Fe3+sites,which promotes the FECO from the volcano-like highest value(88.2%@−0.40 V)to the high plateau(>88.5%@−0.40-−0.60 V),with a much-increased JCO(from 3.24 to 11.23 mA·cm^(−2)).The enhancement is ascribed to the thermodynamically facilitated CO_(2)RR and suppressed competing hydrogen evolution reaction,as well as the kinetically increased electroactive surface area and improved charge transfer,due to the stabilized Fe^(3+)sites and enriched defects by fluorine *** finding provides an efficient strategy to enhance the CO_(2)RR performance of Fe-N-C SSCs by stabilizing Fe^(3+).

关键词： carbon dioxide electroreduction iron-nitrogen-carbon single-site catalysts fluorine-doping active site regulation

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In situ surface-confined fabrication of single atomic Fe-N_(4) on N-doped carbon nanoleaves for oxygen reduction reaction

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Journal of Energy Chemistry 2021年第8期30卷 482-491,I0011页

作者： Xiaojing Jiang Jianian Chen Fenglei Lyu Chen Cheng Qixuan Zhong Xuchun Wang Ayaz Mahsud Liang Zhang Qiao Zhang Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123China

Controllable fabrication of Fe-N-C based single-atom catalysts(SACs)for enhanced electrocatalytic performance is highly desirable but still ***,an in situ surface-confined strategy was demonstrated for the synthesis of single atomic Fe-N_(4))on N-doped carbon nanoleaves(L-FeNC).The in situ generated Zn3[Fe(CN)6]2 could not only serve as a protection layer against collapse of nanoleaves but also provide abundant Fe source for the formation of Fe-N moieties during pyrolysis,leading to high surface area and high graphitization degree of L-FeNC *** from abundant Fe-N_(4))active sites,enhanced mass and charge transfer,the as-prepared L-FeNC manifested a half-wave potential of 0.89 V for oxygen reduction reaction(ORR)in 0.1 M KOH.A maximum power density of 140 m W cm^(-2)and stable discharge voltage even after operation for 50,000 s have been demonstrated when the L-FeNC was used as air cathode for Zn-air *** work not only provided a unique surfaceconfined strategy for the synthesis of two-dimensional nanocarbons,but also demonstrated the significant benefit from rational design and engineering of Fe-N-C SACs,thus offering great opportunities for fabrication of efficient energy conversion and storage devices.

关键词： Single atom catalyst iron-nitrogen-carbon Surface confine Oxygen reduction reaction Metal-organic frameworks

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