Siphumelele Majodina, Ryan Walmsley, Alisa Govender, Eric C. Hosten, Jaco Olivier, Zenixole Tshentu, Adeniyi S. Ogunlaja
{"title":"配体对CoMo/γ-Al2O3表面特性及二苯并噻吩类化合物加氢脱硫催化活性的影响","authors":"Siphumelele Majodina, Ryan Walmsley, Alisa Govender, Eric C. Hosten, Jaco Olivier, Zenixole Tshentu, Adeniyi S. Ogunlaja","doi":"10.1002/open.202400123","DOIUrl":null,"url":null,"abstract":"<p>Refractory sulfur compounds in fuel oils combust, releasing sulfur oxides (SOx) into the atmosphere, which is a significant source of pollution. In this study, we focused on comparing the surface properties and hydrodesulfurization (HDS) activity of CoMo-(L)/γ-Al<sub>2</sub>O<sub>3</sub> containing chelating ligands (L), specifically acetic acid (AA), with those of ethylenediaminetetraacetic acid (EDTA), citric acid (CA). CoMo/γ-Al<sub>2</sub>O<sub>3</sub>, CoMo-AA/γ-Al<sub>2</sub>O<sub>3</sub>, CoMo-EDTA/γ-Al<sub>2</sub>O<sub>3</sub> and CoMo/γ-Al<sub>2</sub>O<sub>3</sub> were prepared by hydrothermal treatment of the mixtures of Co(NO<sub>3</sub>)<sub>2</sub>.6H<sub>2</sub>O and (NH<sub>4</sub>)<sub>6</sub>Mo<sub>7</sub>O<sub>24</sub>.4H<sub>2</sub>O with stoichiometric Co/Mo ratios and enriched with chelating ligands (L=AA, CA and EDTA). Based on the product distributions of the hydrodesulfurization (HDS) of dibenzothiophene (DBT), a reaction pathway of dibenzothiophene (DBT) HDS was proposed to follow hydrogenation (HYD) and direct desulfurization (DDS) routes. In addition, the ligand modification of CoMo/γ-Al<sub>2</sub>O<sub>3</sub> catalysts resulted in enhancement of surface properties and HDS activity which is in the order of CoMo-CA/γ-Al<sub>2</sub>O<sub>3</sub> (98 %)> CoMo-AA/γ-Al<sub>2</sub>O<sub>3</sub> (94 %) > CoMo-EDTA/γ-Al<sub>2</sub>O<sub>3</sub> (90 %) > CoMo/γ-Al<sub>2</sub>O<sub>3</sub> (43 %). CoMo-AA/γ-Al<sub>2</sub>O<sub>3</sub> presented a higher HYD/DDS ratio compared to CoMo-CA/γ-Al<sub>2</sub>O<sub>3</sub>, CoMo-EDTA/γ-Al<sub>2</sub>O<sub>3</sub>, and CoMo/γ-Al<sub>2</sub>O<sub>3</sub>, respectively which makes it a promising HDS catalyst.</p>","PeriodicalId":9831,"journal":{"name":"ChemistryOpen","volume":"14 4","pages":""},"PeriodicalIF":2.5000,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/open.202400123","citationCount":"0","resultStr":"{\"title\":\"Influence of Ligands on the Surface Characteristics of CoMo/γ-Al2O3 and Hydrodesulfurization Catalytic Activity on Dibenzothiophene-Type Compounds\",\"authors\":\"Siphumelele Majodina, Ryan Walmsley, Alisa Govender, Eric C. Hosten, Jaco Olivier, Zenixole Tshentu, Adeniyi S. Ogunlaja\",\"doi\":\"10.1002/open.202400123\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Refractory sulfur compounds in fuel oils combust, releasing sulfur oxides (SOx) into the atmosphere, which is a significant source of pollution. In this study, we focused on comparing the surface properties and hydrodesulfurization (HDS) activity of CoMo-(L)/γ-Al<sub>2</sub>O<sub>3</sub> containing chelating ligands (L), specifically acetic acid (AA), with those of ethylenediaminetetraacetic acid (EDTA), citric acid (CA). CoMo/γ-Al<sub>2</sub>O<sub>3</sub>, CoMo-AA/γ-Al<sub>2</sub>O<sub>3</sub>, CoMo-EDTA/γ-Al<sub>2</sub>O<sub>3</sub> and CoMo/γ-Al<sub>2</sub>O<sub>3</sub> were prepared by hydrothermal treatment of the mixtures of Co(NO<sub>3</sub>)<sub>2</sub>.6H<sub>2</sub>O and (NH<sub>4</sub>)<sub>6</sub>Mo<sub>7</sub>O<sub>24</sub>.4H<sub>2</sub>O with stoichiometric Co/Mo ratios and enriched with chelating ligands (L=AA, CA and EDTA). Based on the product distributions of the hydrodesulfurization (HDS) of dibenzothiophene (DBT), a reaction pathway of dibenzothiophene (DBT) HDS was proposed to follow hydrogenation (HYD) and direct desulfurization (DDS) routes. In addition, the ligand modification of CoMo/γ-Al<sub>2</sub>O<sub>3</sub> catalysts resulted in enhancement of surface properties and HDS activity which is in the order of CoMo-CA/γ-Al<sub>2</sub>O<sub>3</sub> (98 %)> CoMo-AA/γ-Al<sub>2</sub>O<sub>3</sub> (94 %) > CoMo-EDTA/γ-Al<sub>2</sub>O<sub>3</sub> (90 %) > CoMo/γ-Al<sub>2</sub>O<sub>3</sub> (43 %). CoMo-AA/γ-Al<sub>2</sub>O<sub>3</sub> presented a higher HYD/DDS ratio compared to CoMo-CA/γ-Al<sub>2</sub>O<sub>3</sub>, CoMo-EDTA/γ-Al<sub>2</sub>O<sub>3</sub>, and CoMo/γ-Al<sub>2</sub>O<sub>3</sub>, respectively which makes it a promising HDS catalyst.</p>\",\"PeriodicalId\":9831,\"journal\":{\"name\":\"ChemistryOpen\",\"volume\":\"14 4\",\"pages\":\"\"},\"PeriodicalIF\":2.5000,\"publicationDate\":\"2025-03-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://onlinelibrary.wiley.com/doi/epdf/10.1002/open.202400123\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ChemistryOpen\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/open.202400123\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ChemistryOpen","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/open.202400123","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
燃料油中的难熔硫化合物燃烧时，会向大气中释放硫氧化物（SOx），这是一个重要的污染源。在本研究中，我们重点比较了CoMo-(L)/γ-Al2O3含螯合配体(L)，特别是乙酸（AA）与乙二胺四乙酸（EDTA）、柠檬酸（CA）的表面性质和加氢脱硫（HDS）活性。以Co(NO3)2.6H2O和（NH4）6Mo7O24.4H2O为化学量Co/Mo比，用L=AA、CA和EDTA的络合配体对其进行水热处理，制备CoMo/γ-Al2O3、CoMo-AA/γ-Al2O3、CoMo-EDTA/γ-Al2O3和CoMo/γ-Al2O3。根据二苯并噻吩（DBT）加氢脱硫（HDS）的产物分布，提出了二苯并噻吩（DBT）加氢脱硫（HDS）的反应途径，即遵循加氢（HYD）和直接脱硫（DDS）途径。此外，配体修饰的CoMo/γ-Al2O3催化剂的表面性能和HDS活性依次为CoMo- ca /γ-Al2O3 (98%)> CoMo- aa /γ-Al2O3 (94%)> CoMo- edta /γ-Al2O3 (90%)> CoMo/γ-Al2O3（43%）。与CoMo- ca /γ-Al2O3、CoMo- edta /γ-Al2O3和CoMo- γ-Al2O3相比，CoMo- aa /γ-Al2O3具有更高的HYD/DDS比，是一种很有前景的HDS催化剂。
Influence of Ligands on the Surface Characteristics of CoMo/γ-Al2O3 and Hydrodesulfurization Catalytic Activity on Dibenzothiophene-Type Compounds
Refractory sulfur compounds in fuel oils combust, releasing sulfur oxides (SOx) into the atmosphere, which is a significant source of pollution. In this study, we focused on comparing the surface properties and hydrodesulfurization (HDS) activity of CoMo-(L)/γ-Al2O3 containing chelating ligands (L), specifically acetic acid (AA), with those of ethylenediaminetetraacetic acid (EDTA), citric acid (CA). CoMo/γ-Al2O3, CoMo-AA/γ-Al2O3, CoMo-EDTA/γ-Al2O3 and CoMo/γ-Al2O3 were prepared by hydrothermal treatment of the mixtures of Co(NO3)2.6H2O and (NH4)6Mo7O24.4H2O with stoichiometric Co/Mo ratios and enriched with chelating ligands (L=AA, CA and EDTA). Based on the product distributions of the hydrodesulfurization (HDS) of dibenzothiophene (DBT), a reaction pathway of dibenzothiophene (DBT) HDS was proposed to follow hydrogenation (HYD) and direct desulfurization (DDS) routes. In addition, the ligand modification of CoMo/γ-Al2O3 catalysts resulted in enhancement of surface properties and HDS activity which is in the order of CoMo-CA/γ-Al2O3 (98 %)> CoMo-AA/γ-Al2O3 (94 %) > CoMo-EDTA/γ-Al2O3 (90 %) > CoMo/γ-Al2O3 (43 %). CoMo-AA/γ-Al2O3 presented a higher HYD/DDS ratio compared to CoMo-CA/γ-Al2O3, CoMo-EDTA/γ-Al2O3, and CoMo/γ-Al2O3, respectively which makes it a promising HDS catalyst.
期刊介绍：
ChemistryOpen is a multidisciplinary, gold-road open-access, international forum for the publication of outstanding Reviews, Full Papers, and Communications from all areas of chemistry and related fields. It is co-owned by 16 continental European Chemical Societies, who have banded together in the alliance called ChemPubSoc Europe for the purpose of publishing high-quality journals in the field of chemistry and its border disciplines. As some of the governments of the countries represented in ChemPubSoc Europe have strongly recommended that the research conducted with their funding is freely accessible for all readers (Open Access), ChemPubSoc Europe was concerned that no journal for which the ethical standards were monitored by a chemical society was available for such papers. ChemistryOpen fills this gap.
求助内容：
应助结果提醒方式：
京公网安备 11010802042870号
