Zhiyuan Deng , Yinying Shu , Junzheng Qiu , Jianwei Wang , Yunpeng Shi , Minghui Tang , Yahui Cai , Xiaogang Yang , Jundie Hu , Jiafu Qu
{"title":"用于增强二氧化碳加氢制甲酸酯的钯/镍钴氧化物杂化纳米催化剂的抗缺陷工程设计","authors":"Zhiyuan Deng , Yinying Shu , Junzheng Qiu , Jianwei Wang , Yunpeng Shi , Minghui Tang , Yahui Cai , Xiaogang Yang , Jundie Hu , Jiafu Qu","doi":"10.1016/j.jcat.2024.115622","DOIUrl":null,"url":null,"abstract":"<div><p>Efficiently converting CO<sub>2</sub> into value-added chemicals remains a significant challenge due to its inert nature. Here, we present the rational design of Pd/NiCo<sub>2</sub>O<sub>4</sub> hybrid nanocatalysts with diverse morphologies for highly efficient CO<sub>2</sub> hydrogenation to formate. The synergistic combination of Pd and NiCo<sub>2</sub>O<sub>4</sub> offers improved catalytic activity towards formate production. Remarkably, the observation of a morphology-dependent Pd-NiCo<sub>2</sub>O<sub>4</sub> interaction, linked to the presence of oxygen vacancies in NiCo<sub>2</sub>O<sub>4</sub>, significantly contributes to our understanding of catalytic activity. The rose-like Pd/NiCo<sub>2</sub>O<sub>4</sub> catalyst achieves an impressive formate yield (85.3 mol<sub>formate</sub> mol<sub>totalPd</sub><sup>−1</sup> h<sup>−1</sup>) due to its low oxygen vacancy concentration and subsequent generation of less positively-charged Pd species, emphasizing the crucial role of oxygen vacancies in hybrid nanocatalyst performance. These findings were further validated through density functional theory calculations, providing valuable insights into the design and optimization of nanocatalysts for CO<sub>2</sub> hydrogenation. This contributes to the development of efficient and sustainable processes for CO<sub>2</sub> utilization in the production of formate and other valuable chemicals.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Anti-defect engineering of Pd/NiCo2O4 hybrid nanocatalysts for enhanced CO2 hydrogenation to formate\",\"authors\":\"Zhiyuan Deng , Yinying Shu , Junzheng Qiu , Jianwei Wang , Yunpeng Shi , Minghui Tang , Yahui Cai , Xiaogang Yang , Jundie Hu , Jiafu Qu\",\"doi\":\"10.1016/j.jcat.2024.115622\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Efficiently converting CO<sub>2</sub> into value-added chemicals remains a significant challenge due to its inert nature. Here, we present the rational design of Pd/NiCo<sub>2</sub>O<sub>4</sub> hybrid nanocatalysts with diverse morphologies for highly efficient CO<sub>2</sub> hydrogenation to formate. The synergistic combination of Pd and NiCo<sub>2</sub>O<sub>4</sub> offers improved catalytic activity towards formate production. Remarkably, the observation of a morphology-dependent Pd-NiCo<sub>2</sub>O<sub>4</sub> interaction, linked to the presence of oxygen vacancies in NiCo<sub>2</sub>O<sub>4</sub>, significantly contributes to our understanding of catalytic activity. The rose-like Pd/NiCo<sub>2</sub>O<sub>4</sub> catalyst achieves an impressive formate yield (85.3 mol<sub>formate</sub> mol<sub>totalPd</sub><sup>−1</sup> h<sup>−1</sup>) due to its low oxygen vacancy concentration and subsequent generation of less positively-charged Pd species, emphasizing the crucial role of oxygen vacancies in hybrid nanocatalyst performance. These findings were further validated through density functional theory calculations, providing valuable insights into the design and optimization of nanocatalysts for CO<sub>2</sub> hydrogenation. This contributes to the development of efficient and sustainable processes for CO<sub>2</sub> utilization in the production of formate and other valuable chemicals.</p></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-06-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S002195172400335X\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S002195172400335X","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Anti-defect engineering of Pd/NiCo2O4 hybrid nanocatalysts for enhanced CO2 hydrogenation to formate
Efficiently converting CO2 into value-added chemicals remains a significant challenge due to its inert nature. Here, we present the rational design of Pd/NiCo2O4 hybrid nanocatalysts with diverse morphologies for highly efficient CO2 hydrogenation to formate. The synergistic combination of Pd and NiCo2O4 offers improved catalytic activity towards formate production. Remarkably, the observation of a morphology-dependent Pd-NiCo2O4 interaction, linked to the presence of oxygen vacancies in NiCo2O4, significantly contributes to our understanding of catalytic activity. The rose-like Pd/NiCo2O4 catalyst achieves an impressive formate yield (85.3 molformate moltotalPd−1 h−1) due to its low oxygen vacancy concentration and subsequent generation of less positively-charged Pd species, emphasizing the crucial role of oxygen vacancies in hybrid nanocatalyst performance. These findings were further validated through density functional theory calculations, providing valuable insights into the design and optimization of nanocatalysts for CO2 hydrogenation. This contributes to the development of efficient and sustainable processes for CO2 utilization in the production of formate and other valuable chemicals.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.