Nitrogen-doped carbon nanotube-encapsulated nickel nanoparticles assembled on graphene for efficient CO2 electroreduction

Nitrogen-doped carbon nanotube-encapsulated nickel nanoparticles assembled on graphene for efficient CO2 electroreduction
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氮掺杂碳纳米管封装的镍纳米粒子组装在石墨烯上,用于高效 CO2 电还原

DOI:
10.1016/j.cclet.2020.04.056
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发表时间:
2020-05
影响因子:
9.1
通讯作者:
Yang Hou
Yang Hou
中科院分区:
化学1区
文献类型:
--
作者:
Tingting Wang;Jian Yang;Jiayi Chen;Qinggang He;Bin Yang;Lecheng Lei;Han Zhang;Meng Ni;Bin Yang;Yang Hou

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摘要金属纳米粒子包裹的三维纳米碳杂化材料是近年来在实用和经济条件限制下促进CO2电还原反应的新兴催化剂。在此,我们报道了一种一步热解策略,用于制备在石墨烯表面组装的N掺杂碳纳米管(CNT)封装的Ni NPs(N/NiNPs@CNT/G)以有效地将CO2转化为CO。在这种3D混合物中,被五个石墨碳层涂覆的Ni NP的粒度小于100 nm,引入到具有可计数CNT的石墨烯中的N掺杂剂的量被确定为7.27at%。由于独特的CNT封装的Ni NPs结构和N掺杂剂,所获得的N/NiNPs@CNT/G杂化物显示出优异的CRR活性,在-0.7 V下具有97.7%的高法拉第效率和7.9 mA/cm 2的大CO部分电流密度,这优于那些报道的金属NPs负载的碳基CRR电催化剂。此外,在N/NiNPs@CNT/G上观察到134 mV/dec的低Tafel斜率、−0.9 V下387.3 CO/h的转换频率以及长期CRR操作期间的微小性能损失。实验观察表明,由碳层沿着与N掺杂剂封装的Ni NP在具有高电流密度的CO2转化为CO中具有重要意义。
Abstract Exploring 3D hybrid nanocarbons encapsulated with metal nanoparticles (NPs) are recently considered as emerging catalysts for boosting CO2 electroreduction reaction (CRR) under practical and economic limits. Herein, we report a one-step pyrolysis strategy for fabricating N-doped carbon nanotube (CNT)-encapsulated Ni NPs assembled on the surface of graphene (N/NiNPs@CNT/G) to efficiently convert CO2 into CO. In such 3D hybrid, the particle size of Ni NPs that coated by five graphitic carbon layers is less than 100 nm, and the amount of N dopants introduced into graphene with countable CNTs is determined to 7.27 at%. Thanks to unique CNT-encapsulated Ni NPs structure and N dopants, the achieved N/NiNPs@CNT/G hybrid displays an exceptional CRR activity with a high Faradaic efficiency of 97.7% and large CO partial current density of 7.9 mA/cm2 at −0.7 V, which outperforms those reported metallic NPs loaded carbon based CRR electrocatalysts. Further, a low Tafel slope of 134 mV/dec, a turnover frequency of 387.3 CO/h at −0.9 V, and tiny performance losses during long-term CRR operation are observed on N/NiNPs@CNT/G. Experimental observations illustrate that the Ni NPs encapsulated by carbon layers along with N dopants are of great importance in the conversion of CO2 into CO with high current density.
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