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Core-Shell ZIF-8@ZIF-67 Derived CoP Nanoparticles-Embedded N-doped Carbon Nanotube Hollow Polyhedron for Efficient Over-all Water Splitting
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-01-29 , DOI: 10.1021/jacs.7b12420 Yuan Pan 1, 2 , Kaian Sun 2 , Shoujie Liu 1, 3 , Xing Cao 1 , Konglin Wu 1, 3 , Weng-Chon Cheong 1 , Zheng Chen 1 , Yu Wang 1 , Yang Li 1 , Yunqi Liu 2 , Dingsheng Wang 1 , Qing Peng 1 , Chen Chen 1 , Yadong Li 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-01-29 , DOI: 10.1021/jacs.7b12420 Yuan Pan 1, 2 , Kaian Sun 2 , Shoujie Liu 1, 3 , Xing Cao 1 , Konglin Wu 1, 3 , Weng-Chon Cheong 1 , Zheng Chen 1 , Yu Wang 1 , Yang Li 1 , Yunqi Liu 2 , Dingsheng Wang 1 , Qing Peng 1 , Chen Chen 1 , Yadong Li 1
Affiliation
The construction of highly active and stable non-noble-metal electrocatalysts for hydrogen and oxygen evolution reactions is a major challenge for overall water splitting. Herein, we report a novel hybrid nanostructure with CoP nanoparticles (NPs) embedded in a N-doped carbon nanotube hollow polyhedron (NCNHP) through a pyrolysis-oxidation-phosphidation strategy derived from core-shell ZIF-8@ZIF-67. Benefiting from the synergistic effects between highly active CoP NPs and NCNHP, the CoP/NCNHP hybrid exhibited outstanding bifunctional electrocatalytic performances. When the CoP/NCNHP was employed as both the anode and cathode for overall water splitting, a potential as low as 1.64 V was needed to achieve the current density of 10 mA·cm-2, and it still exhibited superior activity after continuously working for 36 h with nearly negligible decay in potential. Density functional theory calculations indicated that the electron transfer from NCNHP to CoP could increase the electronic states of the Co d-orbital around the Fermi level, which could increase the binding strength with H and therefore improve the electrocatalytic performance. The strong stability is attributed to high oxidation resistance of the CoP surface protected by the NCNHP.
中文翻译:
核壳 ZIF-8@ZIF-67 衍生的 CoP 纳米颗粒嵌入 N 掺杂碳纳米管中空多面体,用于高效的整体水分解
构建用于析氢和析氧反应的高活性和稳定的非贵金属电催化剂是整体水分解的主要挑战。在此,我们通过源自核-壳 ZIF-8@ZIF-67 的热解-氧化-磷化策略报告了一种新型混合纳米结构,其中 CoP 纳米颗粒(NP)嵌入 N 掺杂的碳纳米管中空多面体(NCNHP)中。受益于高活性 CoP NPs 和 NCNHP 之间的协同效应,CoP/NCNHP 杂化物表现出出色的双功能电催化性能。当 CoP/NCNHP 用作整个水分解的阳极和阴极时,需要低至 1.64 V 的电位才能实现 10 mA·cm-2 的电流密度,并且在连续工作 36 小时后仍表现出优异的活性,电位衰减几乎可以忽略不计。密度泛函理论计算表明,从 NCNHP 到 CoP 的电子转移可以增加费米能级附近 Co d 轨道的电子态,这可以增加与 H 的结合强度,从而提高电催化性能。强稳定性归因于由 NCNHP 保护的 CoP 表面的高抗氧化性。
更新日期:2018-01-29
中文翻译:
核壳 ZIF-8@ZIF-67 衍生的 CoP 纳米颗粒嵌入 N 掺杂碳纳米管中空多面体,用于高效的整体水分解
构建用于析氢和析氧反应的高活性和稳定的非贵金属电催化剂是整体水分解的主要挑战。在此,我们通过源自核-壳 ZIF-8@ZIF-67 的热解-氧化-磷化策略报告了一种新型混合纳米结构,其中 CoP 纳米颗粒(NP)嵌入 N 掺杂的碳纳米管中空多面体(NCNHP)中。受益于高活性 CoP NPs 和 NCNHP 之间的协同效应,CoP/NCNHP 杂化物表现出出色的双功能电催化性能。当 CoP/NCNHP 用作整个水分解的阳极和阴极时,需要低至 1.64 V 的电位才能实现 10 mA·cm-2 的电流密度,并且在连续工作 36 小时后仍表现出优异的活性,电位衰减几乎可以忽略不计。密度泛函理论计算表明,从 NCNHP 到 CoP 的电子转移可以增加费米能级附近 Co d 轨道的电子态,这可以增加与 H 的结合强度,从而提高电催化性能。强稳定性归因于由 NCNHP 保护的 CoP 表面的高抗氧化性。