Shiyi Wang , Mingsheng Luo , Zhi Yang , Ziyang Zhang , Wenshuai Yang , Ziyuan Li , Xiaoteng Cui , Lingman Xia , Changke Shao
{"title":"原位生长在 rGO 上的 CuCoAl-LDHs 衍生的双金属 Cu-Co 催化剂,用于利用合成气合成酒精","authors":"Shiyi Wang , Mingsheng Luo , Zhi Yang , Ziyang Zhang , Wenshuai Yang , Ziyuan Li , Xiaoteng Cui , Lingman Xia , Changke Shao","doi":"10.1016/j.fuel.2024.133735","DOIUrl":null,"url":null,"abstract":"<div><div>Using a citrate-assisted liquid phase co-precipitation method, a CuCoAl-LDH composite nanomaterial was successfully synthesized in situ on rGO and applied to alcohol synthesis for the first time. Structural characterization and morphological observations indicate that the hybrid material consists of hexagonal LDH nanosheets that are vertically aligned, crossed and densely distributed on the rGO surface. The graphene support significantly promoted the dispersion of LDH and prevented strong interlayer stacking during LDH crystal growth. After optimization of the Co/Cu ratio, the Cu<sub>2</sub>Co<sub>1</sub>/Al<sub>2</sub>O<sub>3</sub>/rGO catalyst exhibited a total alcohol selectivity of 60 %, of which 82 % were C<sub>2+</sub> alcohols, and no deactivation was observed after 100 h of reaction. The addition of the graphene support significantly reduced the particle size of the Cu-Co alloy on the catalyst surface, and the particles were highly dispersed on both the Al<sub>2</sub>O<sub>3</sub> matrix and the rGO surface. This dispersion facilitated strong interactions between the Cu-Co alloy particles, while the high thermal conductivity of graphene effectively suppressed the formation of hotspots. In addition, the well-ordered three-dimensional nanosheet structure of the LDH precursor provides a large specific surface area and highly uniformly dispersed active centers. This structure not only promotes the formation of bridge adsorption sites with high CO dissociation ability, which balances multiple bonding and bridge CO adsorption, but also significantly increases the probability of CO insertion, thereby enhancing the performance of HAS. This study provides an effective method for the preparation of LDH/rGO composites, demonstrating their broad potential application prospects.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"381 ","pages":"Article 133735"},"PeriodicalIF":6.7000,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Bimetallic Cu-Co catalyst derived from in-situ grown CuCoAl-LDHs on rGO for alcohols synthesis from syngas\",\"authors\":\"Shiyi Wang , Mingsheng Luo , Zhi Yang , Ziyang Zhang , Wenshuai Yang , Ziyuan Li , Xiaoteng Cui , Lingman Xia , Changke Shao\",\"doi\":\"10.1016/j.fuel.2024.133735\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Using a citrate-assisted liquid phase co-precipitation method, a CuCoAl-LDH composite nanomaterial was successfully synthesized in situ on rGO and applied to alcohol synthesis for the first time. Structural characterization and morphological observations indicate that the hybrid material consists of hexagonal LDH nanosheets that are vertically aligned, crossed and densely distributed on the rGO surface. The graphene support significantly promoted the dispersion of LDH and prevented strong interlayer stacking during LDH crystal growth. After optimization of the Co/Cu ratio, the Cu<sub>2</sub>Co<sub>1</sub>/Al<sub>2</sub>O<sub>3</sub>/rGO catalyst exhibited a total alcohol selectivity of 60 %, of which 82 % were C<sub>2+</sub> alcohols, and no deactivation was observed after 100 h of reaction. The addition of the graphene support significantly reduced the particle size of the Cu-Co alloy on the catalyst surface, and the particles were highly dispersed on both the Al<sub>2</sub>O<sub>3</sub> matrix and the rGO surface. This dispersion facilitated strong interactions between the Cu-Co alloy particles, while the high thermal conductivity of graphene effectively suppressed the formation of hotspots. In addition, the well-ordered three-dimensional nanosheet structure of the LDH precursor provides a large specific surface area and highly uniformly dispersed active centers. This structure not only promotes the formation of bridge adsorption sites with high CO dissociation ability, which balances multiple bonding and bridge CO adsorption, but also significantly increases the probability of CO insertion, thereby enhancing the performance of HAS. This study provides an effective method for the preparation of LDH/rGO composites, demonstrating their broad potential application prospects.</div></div>\",\"PeriodicalId\":325,\"journal\":{\"name\":\"Fuel\",\"volume\":\"381 \",\"pages\":\"Article 133735\"},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2024-11-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fuel\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0016236124028849\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fuel","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0016236124028849","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Bimetallic Cu-Co catalyst derived from in-situ grown CuCoAl-LDHs on rGO for alcohols synthesis from syngas
Using a citrate-assisted liquid phase co-precipitation method, a CuCoAl-LDH composite nanomaterial was successfully synthesized in situ on rGO and applied to alcohol synthesis for the first time. Structural characterization and morphological observations indicate that the hybrid material consists of hexagonal LDH nanosheets that are vertically aligned, crossed and densely distributed on the rGO surface. The graphene support significantly promoted the dispersion of LDH and prevented strong interlayer stacking during LDH crystal growth. After optimization of the Co/Cu ratio, the Cu2Co1/Al2O3/rGO catalyst exhibited a total alcohol selectivity of 60 %, of which 82 % were C2+ alcohols, and no deactivation was observed after 100 h of reaction. The addition of the graphene support significantly reduced the particle size of the Cu-Co alloy on the catalyst surface, and the particles were highly dispersed on both the Al2O3 matrix and the rGO surface. This dispersion facilitated strong interactions between the Cu-Co alloy particles, while the high thermal conductivity of graphene effectively suppressed the formation of hotspots. In addition, the well-ordered three-dimensional nanosheet structure of the LDH precursor provides a large specific surface area and highly uniformly dispersed active centers. This structure not only promotes the formation of bridge adsorption sites with high CO dissociation ability, which balances multiple bonding and bridge CO adsorption, but also significantly increases the probability of CO insertion, thereby enhancing the performance of HAS. This study provides an effective method for the preparation of LDH/rGO composites, demonstrating their broad potential application prospects.
期刊介绍:
The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.