Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO2,ChemSusChem

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Confining Chainmail‐Bearing Ni Nanoparticles in N‐doped Carbon Nanotubes for Robust and Efficient Electroreduction of CO2
ChemSusChem ( IF 7.5 ) Pub Date : 2021-01-19 , DOI: 10.1002/cssc.202002596
Yongjian Niu ₁ , Chunhua Zhang ₂ , Yuanyuan Wang ₁ , Dong Fang ₁ , Linlin Zhang ₁ , Cheng Wang ₁

Affiliation

It still remains challenging to simultaneously achieve high stability, selectivity, and activity in CO₂ reduction. Herein, a dual chainmail‐bearing nickel‐based catalyst (Ni@NC@NCNT) was fabricated via a solvothermal‐evaporation‐calcination approach. In situ encapsulated N‐doped carbon layers (NCs) and nanotubes (NCNTs) gave a dual protection to the metallic core. The confined space well maintained the local alkaline pH value and suppressed hydrogen evolution. Large surface area and abundant pyridinic N and Ni^δ+ sites ensured high CO₂ adsorption capacity and strength. Benefitting from these, it delivered a CO faradaic efficiency of 94.1 % and current density of 48.0 mA cm⁻² at −0.75 and −1.10 V, respectively. Moreover, the performance remained unchanged after continuous electrolysis for 43 h, far exceeding Ni@NC with single chainmail, Ni@NC/NCNT with Ni@NC sitting on the walls of NCNT, bare NCNT and most state‐of‐the‐art catalysts, demonstrating structural superiority of Ni@NC@NCNT. This work sheds light on designing unique architectures to improve electrochemical performances.

中文翻译：

在N掺杂的碳纳米管中限制含链邮的Ni纳米颗粒，以实现鲁棒且有效的CO2电还原

同时实现高稳定性，选择性和降低CO _2的活性仍然具有挑战性。在此，通过溶剂热蒸发煅烧方法制备了一种双链甲负载镍基催化剂（Ni @ NC @ NCNT）。原位封装的N掺杂碳层（NC）和纳米管（NCNT）为金属核提供了双重保护。密闭空间很好地保持了局部碱性pH值并抑制了氢的释放。较大的表面积和丰富的吡啶吡啶N和^{Niδ +}位确保了较高的CO ₂吸附能力和强度。受益于这些，它提供了94.1％的CO法拉第效率和48.0 mA cm ^-2的电流密度分别在-0.75和-1.10 V下。此外，连续电解43小时后，性能仍保持不变，远远超过了使用单链邮件的Ni @ NC，超过了NiCNT壁厚的Ni @ NC / NCNT，位于裸露的NCNT和大多数先进催化剂上的Ni @ NC ，证明了Ni @ NC @ NCNT的结构优势。这项工作为设计独特的体系结构以改善电化学性能提供了启示。

更新日期：2021-02-18

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