Yufei Cui , Hui Yang , Wenhao Zhou , Yongqing Ma , Ganhong Zheng , Bin Chen , Chuhong Zhu , Meiling Wang
{"title":"在 Ni/CeO2 纳米棒上 100% 选择性地将甲烷转化为 C1 产品","authors":"Yufei Cui , Hui Yang , Wenhao Zhou , Yongqing Ma , Ganhong Zheng , Bin Chen , Chuhong Zhu , Meiling Wang","doi":"10.1016/j.jcat.2024.115546","DOIUrl":null,"url":null,"abstract":"<div><p>Selective CH<sub>4</sub> upgrading to C1 products and avoiding over oxidation remains a key challenge. Here, we develop a highly efficient Ni/CeO<sub>2</sub> nanorods containing both uniformly dispersed Ni-single-site and NiO<sub>x</sub>/CeO<sub>2</sub> heterojunction for 100 % selectively CH<sub>4</sub> conversion to C1 products (CH<sub>3</sub>OH, HCHO, CH<sub>3</sub>OOH and HCOOH). Under optimized photocatalytic experimental conditions, a high C1 product yield of 5.6 mmol g<sup>-1</sup>h<sup>−1</sup> was obtained with 100 % selectivity with presence of H<sub>2</sub>O<sub>2</sub>. Mechanism study showed that the Ni-single-site together with formed oxygen vacancy (O<sub>v</sub>) facilitated CH<sub>4</sub> adsorption and activation. The terminal O atom of adsorbed ·OOH can fill the O<sub>v</sub>, with the remaining *OH initiating *CH<sub>3</sub> dehydrogenation and forming *CH<sub>2</sub>OH, which further reacts with ·OH to generate the main product HCHO. During the whole photocatalytic process, the formed NiO<sub>x</sub>/CeO<sub>2</sub> heterojunction promoted carrier separation and enhanced catalytic performance.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":null,"pages":null},"PeriodicalIF":6.5000,"publicationDate":"2024-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"100% selective methane conversion to C1 products over Ni/CeO2 nanorods\",\"authors\":\"Yufei Cui , Hui Yang , Wenhao Zhou , Yongqing Ma , Ganhong Zheng , Bin Chen , Chuhong Zhu , Meiling Wang\",\"doi\":\"10.1016/j.jcat.2024.115546\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Selective CH<sub>4</sub> upgrading to C1 products and avoiding over oxidation remains a key challenge. Here, we develop a highly efficient Ni/CeO<sub>2</sub> nanorods containing both uniformly dispersed Ni-single-site and NiO<sub>x</sub>/CeO<sub>2</sub> heterojunction for 100 % selectively CH<sub>4</sub> conversion to C1 products (CH<sub>3</sub>OH, HCHO, CH<sub>3</sub>OOH and HCOOH). Under optimized photocatalytic experimental conditions, a high C1 product yield of 5.6 mmol g<sup>-1</sup>h<sup>−1</sup> was obtained with 100 % selectivity with presence of H<sub>2</sub>O<sub>2</sub>. Mechanism study showed that the Ni-single-site together with formed oxygen vacancy (O<sub>v</sub>) facilitated CH<sub>4</sub> adsorption and activation. The terminal O atom of adsorbed ·OOH can fill the O<sub>v</sub>, with the remaining *OH initiating *CH<sub>3</sub> dehydrogenation and forming *CH<sub>2</sub>OH, which further reacts with ·OH to generate the main product HCHO. During the whole photocatalytic process, the formed NiO<sub>x</sub>/CeO<sub>2</sub> heterojunction promoted carrier separation and enhanced catalytic performance.</p></div>\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2024-05-13\",\"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/S0021951724002598\",\"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/S0021951724002598","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
100% selective methane conversion to C1 products over Ni/CeO2 nanorods
Selective CH4 upgrading to C1 products and avoiding over oxidation remains a key challenge. Here, we develop a highly efficient Ni/CeO2 nanorods containing both uniformly dispersed Ni-single-site and NiOx/CeO2 heterojunction for 100 % selectively CH4 conversion to C1 products (CH3OH, HCHO, CH3OOH and HCOOH). Under optimized photocatalytic experimental conditions, a high C1 product yield of 5.6 mmol g-1h−1 was obtained with 100 % selectivity with presence of H2O2. Mechanism study showed that the Ni-single-site together with formed oxygen vacancy (Ov) facilitated CH4 adsorption and activation. The terminal O atom of adsorbed ·OOH can fill the Ov, with the remaining *OH initiating *CH3 dehydrogenation and forming *CH2OH, which further reacts with ·OH to generate the main product HCHO. During the whole photocatalytic process, the formed NiOx/CeO2 heterojunction promoted carrier separation and enhanced catalytic performance.
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.
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