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Enhanced Electrocatalytic Activity of Mo-Doped NiFe Layered Double Hydroxide Nanosheet Arrays for the Hydrogen Evolution Reaction
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2022-12-21 , DOI: 10.1021/acsanm.2c04519 Jiawei Guo 1 , Kun Wang 1 , Heng Zhang 1 , Hui Zhang 1
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2022-12-21 , DOI: 10.1021/acsanm.2c04519 Jiawei Guo 1 , Kun Wang 1 , Heng Zhang 1 , Hui Zhang 1
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NiFeMo layered double hydroxide (NiFeMo-LDH) nanosheet array structures in situ grown on Ni foam were rationally designed and fabricated by a convenient and green hydrothermal strategy. The systematic characterization proved that NixFe1Mo1-LDH/NF (x = 4, 6, 8, 10) composites grew on the surface of Ni foam as vertically interlaced LDH nanosheets. The electrochemical results showed that all composites possessed high electrocatalytic activity, and Ni6Fe1Mo1-LDH/NF exhibited the best hydrogen evolution reaction (HER) performance. Furthermore, the nanosheet array structure with the best active metal molar ratio was in situ grown on reduced graphene oxide (rGO) uniformly modified Ni foam (∼210 nm × 20 nm) with an overpotential of 90 mV at 10 cm–2 in an alkaline solution, which was superior to most non-noble metal-based catalysts. Experimental results and density functional theory with the Hubbard U (DFT + U) calculations confirmed that the active site for H adsorption changed from the Fe site to the Mo site after Mo doping in NiFe-LDH, which reduced the water dissociation energy barrier and the subsequent proton adsorption energy barrier and adjusted the electronic structure of Fe and Ni sites, thereby greatly promoting the whole Volmer–Heyrovsky process under alkaline conditions and improving the HER performance. The synergistic coupling of NiFeMo-LDH nanosheets with rGO enhanced conductivity and electrochemical performance. The growth of NiFeMo-LDH on rGO/NF facilitated the formation of bubbles and significantly improved electrochemical stability. The present electronic regulation strategies using metal doping can be extended to synthesize other types of transition metal composite catalysts and used for the development of renewable and friendly energy devices.
中文翻译：
Mo 掺杂 NiFe 层状双氢氧化物纳米片阵列对析氢反应的增强电催化活性
在泡沫镍上原位生长的 NiFeMo 层状双氢氧化物 (NiFeMo-LDH) 纳米片阵列结构是通过一种方便且绿色的水热策略合理设计和制造的。系统表征证明，Ni x Fe 1 Mo 1 -LDH/NF ( x = 4, 6, 8, 10) 复合材料在泡沫镍表面生长为垂直交错的LDH 纳米片。电化学结果表明，所有复合材料均具有较高的电催化活性，Ni 6 Fe 1 Mo 1-LDH/NF表现出最好的析氢反应（HER）性能。此外，具有最佳活性金属摩尔比的纳米片阵列结构原位生长在还原氧化石墨烯 (rGO) 均匀改性的镍泡沫 (~210 nm × 20 nm) 上，在 10 cm –2的碱性溶液中过电位为 90 mV溶液，优于大多数非贵金属基催化剂。哈伯德U的实验结果和密度泛函理论(DFT + U)计算证实，在NiFe-LDH中掺杂Mo后，H吸附活性位点由Fe位点变为Mo位点，降低了水解离能垒和随后的质子吸附能垒，调整了Fe和Ni的电子结构位点，从而极大地促进了碱性条件下整个 Volmer-Heyrovsky 过程，提高了 HER 性能。NiFeMo-LDH 纳米片与 rGO 的协同耦合增强了导电性和电化学性能。NiFeMo-LDH 在 rGO/NF 上的生长促进了气泡的形成并显着提高了电化学稳定性。
更新日期：2022-12-21
中文翻译：
Mo 掺杂 NiFe 层状双氢氧化物纳米片阵列对析氢反应的增强电催化活性
在泡沫镍上原位生长的 NiFeMo 层状双氢氧化物 (NiFeMo-LDH) 纳米片阵列结构是通过一种方便且绿色的水热策略合理设计和制造的。系统表征证明，Ni x Fe 1 Mo 1 -LDH/NF ( x = 4, 6, 8, 10) 复合材料在泡沫镍表面生长为垂直交错的LDH 纳米片。电化学结果表明，所有复合材料均具有较高的电催化活性，Ni 6 Fe 1 Mo 1-LDH/NF表现出最好的析氢反应（HER）性能。此外，具有最佳活性金属摩尔比的纳米片阵列结构原位生长在还原氧化石墨烯 (rGO) 均匀改性的镍泡沫 (~210 nm × 20 nm) 上，在 10 cm –2的碱性溶液中过电位为 90 mV溶液，优于大多数非贵金属基催化剂。哈伯德U的实验结果和密度泛函理论(DFT + U)计算证实，在NiFe-LDH中掺杂Mo后，H吸附活性位点由Fe位点变为Mo位点，降低了水解离能垒和随后的质子吸附能垒，调整了Fe和Ni的电子结构位点，从而极大地促进了碱性条件下整个 Volmer-Heyrovsky 过程，提高了 HER 性能。NiFeMo-LDH 纳米片与 rGO 的协同耦合增强了导电性和电化学性能。NiFeMo-LDH 在 rGO/NF 上的生长促进了气泡的形成并显着提高了电化学稳定性。
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