Suryamol Nambyaruveettil , Labeeb Ali , Mirza Belal Beg , Abbas Khaleel , Mohammednoor Altarawneh
{"title":"一种新型镍沸石-生物炭绿色催化剂:TPR、TPD和XPS研究表明其组成和制备策略优化","authors":"Suryamol Nambyaruveettil , Labeeb Ali , Mirza Belal Beg , Abbas Khaleel , Mohammednoor Altarawneh","doi":"10.1016/j.mseb.2025.118566","DOIUrl":null,"url":null,"abstract":"<div><div>The development in green hydrogenation technology depends on the production of robust and reasonably priced catalyst supports. This study synthesized and optimized a novel Ni-zeolite-biochar hybrid catalyst, improved by changes in composition, method of synthesis, and metal loading. The catalyst was developed using commercially obtained mordenite zeolite with a high-silica framework-type material known for its strong acidity and thermal stability, and biochar derived from date pit powder through controlled pyrolysis, providing acidity and surface oxygenation functionalities, respectively. The investigation of reducibility, metal dispersion, metal support interaction strength and electronic interactions of the material was conducted using temperature-programmed reduction (TPR), temperature-programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS), thereby fully describing it. Out of different nickel loading (5 %,15 %,25 %), 15 % was identified as optimal. Similarly, the effects of zeolite content, impregnation order, and the roles of wet impregnation and co-impregnation in catalyst reducibility were critically analyzed. The best formulation of Nickel zeolite biochar (NZB) exhibited a low reduction temperature (Tmax = 390 °C), high hydrogen consumption (7135.2 μmolg-1), medium metal-support interaction, and high dispersion (63.27 %). Compared to conventional Ni-based catalysts such as Ni/Al<sub>2</sub>O<sub>3</sub> and Ni/SiO<sub>2</sub>, the hybrid system demonstrated an improved reducibility and high metal dispersion. The robustness of the system was enhanced by the acidity of the zeolite and the oxygenation properties of the biochar together. The Ni 2<em>p</em> binding energy exhibited a positive shift on the XPS test, therefore confirming a strong electrical link between the metal and the substrate. This work presents a fresh, environmentally friendly, flexible catalytic support system that enhances nickel dispersion and reducibility. This study will provide the foundation for catalytic applications including selective hydrogenations. The catalytic relevance of the optimized NZB system was demonstrated through its successful application in 1,3-butadiene selective hydrogenation, achieving 100 % conversion with excellent deactivation resistance.</div></div>","PeriodicalId":18233,"journal":{"name":"Materials Science and Engineering: B","volume":"321 ","pages":"Article 118566"},"PeriodicalIF":3.9000,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"A novel Ni–zeolite–biochar green catalyst: optimization of composition and preparation strategy revealed by TPR, TPD, and XPS\",\"authors\":\"Suryamol Nambyaruveettil , Labeeb Ali , Mirza Belal Beg , Abbas Khaleel , Mohammednoor Altarawneh\",\"doi\":\"10.1016/j.mseb.2025.118566\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The development in green hydrogenation technology depends on the production of robust and reasonably priced catalyst supports. This study synthesized and optimized a novel Ni-zeolite-biochar hybrid catalyst, improved by changes in composition, method of synthesis, and metal loading. The catalyst was developed using commercially obtained mordenite zeolite with a high-silica framework-type material known for its strong acidity and thermal stability, and biochar derived from date pit powder through controlled pyrolysis, providing acidity and surface oxygenation functionalities, respectively. The investigation of reducibility, metal dispersion, metal support interaction strength and electronic interactions of the material was conducted using temperature-programmed reduction (TPR), temperature-programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS), thereby fully describing it. Out of different nickel loading (5 %,15 %,25 %), 15 % was identified as optimal. Similarly, the effects of zeolite content, impregnation order, and the roles of wet impregnation and co-impregnation in catalyst reducibility were critically analyzed. The best formulation of Nickel zeolite biochar (NZB) exhibited a low reduction temperature (Tmax = 390 °C), high hydrogen consumption (7135.2 μmolg-1), medium metal-support interaction, and high dispersion (63.27 %). Compared to conventional Ni-based catalysts such as Ni/Al<sub>2</sub>O<sub>3</sub> and Ni/SiO<sub>2</sub>, the hybrid system demonstrated an improved reducibility and high metal dispersion. The robustness of the system was enhanced by the acidity of the zeolite and the oxygenation properties of the biochar together. The Ni 2<em>p</em> binding energy exhibited a positive shift on the XPS test, therefore confirming a strong electrical link between the metal and the substrate. This work presents a fresh, environmentally friendly, flexible catalytic support system that enhances nickel dispersion and reducibility. This study will provide the foundation for catalytic applications including selective hydrogenations. The catalytic relevance of the optimized NZB system was demonstrated through its successful application in 1,3-butadiene selective hydrogenation, achieving 100 % conversion with excellent deactivation resistance.</div></div>\",\"PeriodicalId\":18233,\"journal\":{\"name\":\"Materials Science and Engineering: B\",\"volume\":\"321 \",\"pages\":\"Article 118566\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-06-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Materials Science and Engineering: B\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0921510725005902\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Science and Engineering: B","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0921510725005902","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
A novel Ni–zeolite–biochar green catalyst: optimization of composition and preparation strategy revealed by TPR, TPD, and XPS
The development in green hydrogenation technology depends on the production of robust and reasonably priced catalyst supports. This study synthesized and optimized a novel Ni-zeolite-biochar hybrid catalyst, improved by changes in composition, method of synthesis, and metal loading. The catalyst was developed using commercially obtained mordenite zeolite with a high-silica framework-type material known for its strong acidity and thermal stability, and biochar derived from date pit powder through controlled pyrolysis, providing acidity and surface oxygenation functionalities, respectively. The investigation of reducibility, metal dispersion, metal support interaction strength and electronic interactions of the material was conducted using temperature-programmed reduction (TPR), temperature-programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS), thereby fully describing it. Out of different nickel loading (5 %,15 %,25 %), 15 % was identified as optimal. Similarly, the effects of zeolite content, impregnation order, and the roles of wet impregnation and co-impregnation in catalyst reducibility were critically analyzed. The best formulation of Nickel zeolite biochar (NZB) exhibited a low reduction temperature (Tmax = 390 °C), high hydrogen consumption (7135.2 μmolg-1), medium metal-support interaction, and high dispersion (63.27 %). Compared to conventional Ni-based catalysts such as Ni/Al2O3 and Ni/SiO2, the hybrid system demonstrated an improved reducibility and high metal dispersion. The robustness of the system was enhanced by the acidity of the zeolite and the oxygenation properties of the biochar together. The Ni 2p binding energy exhibited a positive shift on the XPS test, therefore confirming a strong electrical link between the metal and the substrate. This work presents a fresh, environmentally friendly, flexible catalytic support system that enhances nickel dispersion and reducibility. This study will provide the foundation for catalytic applications including selective hydrogenations. The catalytic relevance of the optimized NZB system was demonstrated through its successful application in 1,3-butadiene selective hydrogenation, achieving 100 % conversion with excellent deactivation resistance.
期刊介绍:
The journal provides an international medium for the publication of theoretical and experimental studies and reviews related to the electronic, electrochemical, ionic, magnetic, optical, and biosensing properties of solid state materials in bulk, thin film and particulate forms. Papers dealing with synthesis, processing, characterization, structure, physical properties and computational aspects of nano-crystalline, crystalline, amorphous and glassy forms of ceramics, semiconductors, layered insertion compounds, low-dimensional compounds and systems, fast-ion conductors, polymers and dielectrics are viewed as suitable for publication. Articles focused on nano-structured aspects of these advanced solid-state materials will also be considered suitable.