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Mediating heterogenized nickel phthalocyanine into isolated Ni-N3 moiety for improving activity and stability of electrocatalytic CO2 reduction
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-08-03 , DOI: 10.1016/j.apcatb.2022.121813
Shanhe Gong , Wenbo Wang , Runqing Lu , Minghui Zhu , Haotan Wang , Yun Zhang , Jimin Xie , Chundu Wu , Jun Liu , Mengxian Li , Shouyan Shao , Guisheng Zhu , Xiaomeng Lv

The poor stability of heterogenized nickel phthalocyanine (NiPc) has hindered its application as a desirable catalyst for electrocatalytic carbon dioxide reduction. Herein, the electrocatalytic stability of heterogenized NiPc on nitrogen-doped hollow carbon nanospheres (NiPc@NHCSs) can be optimized via mediating NiPc into Ni-NC moiety (Ni-NC/NHCSs-Y) to construct a stable Ni catalytic unit. Different from the poor activity of NiPc@NHCSs (CO Faradaic efficiency, FECO< 80%, stability < 1200 s), the optimal catalyst (Ni-NC/NHCSs-600) with unsaturated Ni-N3 nitrogen-vacancy structure, displays FECO of 98.57% and CO turnover frequency of 3.75 s−1 at − 0.87 V vs. RHE, and stable operation over 14 h (−0.82 V vs. RHE). The stabilization mechanism and the temperature effect on the structure-activity relationship are systematically explored, which successfully steers the design of stable Ni-NC catalytic unit on different carbon substrate, while a zinc-CO2 rechargeable battery is constructed, displaying a peak power density of 0.64 mW cm−2 and FECO of 91.45%.



中文翻译:

将异质化镍酞菁介导到分离的 Ni-N3 部分以提高电催化 CO2 还原的活性和稳定性

异质化镍酞菁(NiPc)稳定性差,阻碍了其作为电催化二氧化碳还原催化剂的应用。在此,可以通过将NiPc介导到Ni-NC部分(Ni-NC/NHCSs- Y )中来优化异质NiPc在氮掺杂中空碳纳米球(NiPc@NHCSs)上的电催化稳定性,以构建稳定的Ni催化单元。不同于 NiPc@NHCSs 的活性差(CO 法拉第效率,FEC< 80%, 稳定性 < 1200 s), 具有不饱和 Ni-N 3氮空位结构的最佳催化剂 (Ni-NC/NHCSs-600), 展示FEC为 98.57%,CO 周转频率为 3.75 s -1在 - 0.87 V vs。RHE,并在 14 小时内稳定运行(-0.82 VRHE)。系统地探讨了稳定机制和温度对构效关系的影响,成功指导了在不同碳基底上稳定的 Ni-NC 催化单元的设计,同时构建了具有峰值功率密度的锌-CO 2可充电电池0.64 mW cm -2FE一氧化碳91.45%。

更新日期:2022-08-03
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