{"title":"锌蒸发诱导形成所需的镍纳米颗粒并包裹超薄碳壳,用于高效电催化制取与甲醇升级耦合的 H2","authors":"Kexian Hou, Shizhen Zhang, Peng Yin, Tao Liu, Yanfeng Cao, Mingxi Wang, Weiting Zhan, Ling Wu","doi":"10.1021/acsami.4c10405","DOIUrl":null,"url":null,"abstract":"The integration of the hydrogen evolution reaction (HER) with the methanol oxidation reaction (MOR) has been demonstrated to be a viable strategy for the energy-saving generation of H<sub>2</sub> and value-added formate, which relies primarily on highly active and cost-effective bifunctional electrocatalysts. Herein, an efficient electrocatalyst consisting of controllable Ni nanoparticles (NPs) coated with ultrathin graphitic carbon shells was obtained by the pyrolysis of a Ni–Zn metal–organic framework. Intriguingly, we found that zinc vaporization not only resulted in the relatively small Ni NPs but also ultrathin carbon shells (≤3 layers). The density functional theory simulations confirmed that these ultrathin carbon shells significantly influenced electrocatalytic activity by facilitating electron transfer from the Ni core to the carbon shell. The optimized Ni<sub>1</sub>(Zn)@C demonstrated high catalytic activity for both HER and MOR, and only a low potential of 97 mV at 10 mA cm<sup>–2</sup> was required for HER and 1.48 V at 30 mA cm<sup>–2</sup> for MOR. In a two-electrode electrocatalytic cell measurement, a cell voltage of 1.63 V was observed at 10 mA cm<sup>–2</sup> in the presence of methanol, 240 mV lower than that without methanol.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3000,"publicationDate":"2024-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Zinc Vaporization Induced Formation of Desired Ni Nanoparticles Coated with Ultrathin Carbon Shells for Efficient Electrocatalytic H2 Production Coupling with Methanol Upgrading\",\"authors\":\"Kexian Hou, Shizhen Zhang, Peng Yin, Tao Liu, Yanfeng Cao, Mingxi Wang, Weiting Zhan, Ling Wu\",\"doi\":\"10.1021/acsami.4c10405\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The integration of the hydrogen evolution reaction (HER) with the methanol oxidation reaction (MOR) has been demonstrated to be a viable strategy for the energy-saving generation of H<sub>2</sub> and value-added formate, which relies primarily on highly active and cost-effective bifunctional electrocatalysts. Herein, an efficient electrocatalyst consisting of controllable Ni nanoparticles (NPs) coated with ultrathin graphitic carbon shells was obtained by the pyrolysis of a Ni–Zn metal–organic framework. Intriguingly, we found that zinc vaporization not only resulted in the relatively small Ni NPs but also ultrathin carbon shells (≤3 layers). The density functional theory simulations confirmed that these ultrathin carbon shells significantly influenced electrocatalytic activity by facilitating electron transfer from the Ni core to the carbon shell. The optimized Ni<sub>1</sub>(Zn)@C demonstrated high catalytic activity for both HER and MOR, and only a low potential of 97 mV at 10 mA cm<sup>–2</sup> was required for HER and 1.48 V at 30 mA cm<sup>–2</sup> for MOR. In a two-electrode electrocatalytic cell measurement, a cell voltage of 1.63 V was observed at 10 mA cm<sup>–2</sup> in the presence of methanol, 240 mV lower than that without methanol.\",\"PeriodicalId\":5,\"journal\":{\"name\":\"ACS Applied Materials & Interfaces\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.3000,\"publicationDate\":\"2024-09-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Materials & Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsami.4c10405\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Materials & Interfaces","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsami.4c10405","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
氢气进化反应(HER)与甲醇氧化反应(MOR)的结合已被证明是生成 H2 和增值甲酸盐的可行节能策略,这主要依赖于高活性和高成本效益的双功能电催化剂。在此,我们通过热解镍锌金属有机框架,获得了一种高效的电催化剂,它由可控的镍纳米颗粒(NPs)和超薄石墨碳壳组成。有趣的是,我们发现锌蒸发不仅产生了相对较小的镍纳米粒子,还产生了超薄碳壳(≤3 层)。密度泛函理论模拟证实,这些超薄碳壳可促进电子从镍核转移到碳壳,从而显著影响电催化活性。优化后的 Ni1(Zn)@C 对 HER 和 MOR 都表现出很高的催化活性,HER 在 10 mA cm-2 下只需要 97 mV 的低电位,MOR 在 30 mA cm-2 下需要 1.48 V 的低电位。在双电极电催化电池测量中,在有甲醇存在的情况下,10 mA cm-2 时电池电压为 1.63 V,比没有甲醇时低 240 mV。
Zinc Vaporization Induced Formation of Desired Ni Nanoparticles Coated with Ultrathin Carbon Shells for Efficient Electrocatalytic H2 Production Coupling with Methanol Upgrading
The integration of the hydrogen evolution reaction (HER) with the methanol oxidation reaction (MOR) has been demonstrated to be a viable strategy for the energy-saving generation of H2 and value-added formate, which relies primarily on highly active and cost-effective bifunctional electrocatalysts. Herein, an efficient electrocatalyst consisting of controllable Ni nanoparticles (NPs) coated with ultrathin graphitic carbon shells was obtained by the pyrolysis of a Ni–Zn metal–organic framework. Intriguingly, we found that zinc vaporization not only resulted in the relatively small Ni NPs but also ultrathin carbon shells (≤3 layers). The density functional theory simulations confirmed that these ultrathin carbon shells significantly influenced electrocatalytic activity by facilitating electron transfer from the Ni core to the carbon shell. The optimized Ni1(Zn)@C demonstrated high catalytic activity for both HER and MOR, and only a low potential of 97 mV at 10 mA cm–2 was required for HER and 1.48 V at 30 mA cm–2 for MOR. In a two-electrode electrocatalytic cell measurement, a cell voltage of 1.63 V was observed at 10 mA cm–2 in the presence of methanol, 240 mV lower than that without methanol.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.