燃料化学学报Pub Date : 2024-11-01DOI: 10.1016/S1872-5813(24)60463-9
Pu DAI , Mengya GUO , Hui GE , Caimei FAN , Xuekuan LI , Rui LI , Mingxing TANG
{"title":"Preparation of Ni/ZnCo2O4@ZnO composite metal oxide adsorbent and its adsorption desulfurization and regeneration performance","authors":"Pu DAI , Mengya GUO , Hui GE , Caimei FAN , Xuekuan LI , Rui LI , Mingxing TANG","doi":"10.1016/S1872-5813(24)60463-9","DOIUrl":"10.1016/S1872-5813(24)60463-9","url":null,"abstract":"<div><div>Metal Co was introduced into ZnO by co-precipitation to form composite metal oxides as the desulfurization agent with different Co contents, with which the desulfurization activity and regeneration performance were investigated. The systematic characterization of the structure and properties of the desulfurization agent using XRD, TEM, N<sub>2</sub> adsorption and desorption, XPS and H<sub>2</sub>-TPR confirmed that the composite metal oxide desulfurization agent had the Ni/ZnCo<sub>2</sub>O<sub>4</sub>@ZnO structure. The formation of ZnCo<sub>2</sub>O<sub>4</sub> in the composite metal oxides desulfurization agent facilitated the particle size reduction, dispersion enhancement and specific surface area increase of the desulfurization agent, which also acted as an adsorbent for H<sub>2</sub>S indicated by the XRD analysis, improving the sulfur adsorption capacity of the desulfurization agent. The desulfurization performance of all the composite metal oxide desulfurization agents was higher than that of Ni/ZnO, in which the desulfurization agent NZCo-3 with a molar ratio of Zn:Co of 1:1 exhibited the optimal desulfurization performance, and the desulfurization rate was 100% at a reaction temperature of 300 °C, a hydrogen pressure of 3 MPa, a mass-air velocity of 2.2 h<sup>–1</sup>, and a hydrogen-oil ratio of 300, and the excellent desulfurization performance was maintained after 6 cycles. The results of this study provide new ideas for the rational design of Ni/ZnO desulfurization agent to improve its desulfurization and regeneration performance.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 11","pages":"Pages 1706-1714"},"PeriodicalIF":0.0,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723037","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-11-01DOI: 10.1016/S1872-5813(24)60493-7
Yiming LIU , Jingjing MIAO , Wanggang ZHANG , Aili WEI , Jian WANG
{"title":"In-situ photodeposition of co-catalyst Ni2P on CdS for photocatalytic conversion of ethanol for synergistic hydrogen production","authors":"Yiming LIU , Jingjing MIAO , Wanggang ZHANG , Aili WEI , Jian WANG","doi":"10.1016/S1872-5813(24)60493-7","DOIUrl":"10.1016/S1872-5813(24)60493-7","url":null,"abstract":"<div><div>In this study, Ni<sub>2</sub>P/CdS composites were constructed by depositing non-precious metal co-catalyst Ni<sub>2</sub>P on a one-dimensional network of CdS using a simple <em>in-situ</em> photodeposition method. The prepared photocatalysts promoted the decomposition of ethanol into high-value-added products while generating hydrogen. The composite photoanodes loaded with the Ni<sub>2</sub>P co-catalysts showed significantly higher ethanol conversion and hydrogen production in the visible light region, which was almost three times higher than that of pure CdS. The main products of photocatalytic ethanol production are acetaldehyde (AA) and 2,3-butanediol (2,3-BDA). Compared with CdS, the selectivity of the composite photocatalysts for converting ethanol to acetaldehyde was significantly improved (62% to 78%). Characterization of the prepared photocatalysts confirmed that the loading of Ni<sub>2</sub>P co-catalysts on CdS not only broadened the optical region of the catalysts for trapping light but also effectively promoted the separation and transfer of charge carriers, which significantly improved the photocatalytic efficiency of ethanol conversion and hydrogen production in the catalysts. It has been proven through Electron Paramagnetic Resonance testing that loading a Ni<sub>2</sub>P co-catalyst on CdS is beneficial for the adsorption of hydroxyethyl radicals (*CH(OH)CH<sub>3</sub>), thereby further improving the selectivity of acetaldehyde. This study plays an important role in the rational design of composite catalyst structures and the introduction of co-catalysts to improve catalyst performance, promote green chemistry, advocate a low-carbon society, and promote sustainable development.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 11","pages":"Pages 1629-1640"},"PeriodicalIF":0.0,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723034","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-11-01DOI: 10.1016/S1872-5813(24)60464-0
Xin ZHANG , Guoqiang LI , Mei HONG , Hongyan BAN , Lixia YANG , Xingchen LIU , Feng LI , Ekaterina Vladimirovna Matus , Congming LI , Lei LI
{"title":"Development of Nix/Mg1–x-MOF-74 for highly efficient CO2/N2 separation","authors":"Xin ZHANG , Guoqiang LI , Mei HONG , Hongyan BAN , Lixia YANG , Xingchen LIU , Feng LI , Ekaterina Vladimirovna Matus , Congming LI , Lei LI","doi":"10.1016/S1872-5813(24)60464-0","DOIUrl":"10.1016/S1872-5813(24)60464-0","url":null,"abstract":"<div><div>To enhance the separation selectivity of Mg-MOF-74 towards CO<sub>2</sub> in a CO<sub>2</sub>/N<sub>2</sub> mixture, a series of Mg-MOF-74 and Ni<sub><em>x</em></sub>/Mg<sub>1–<em>x</em></sub>-MOF-74 adsorbents were prepared by solvothermal synthesis in this paper. It was found that the adsorption capacity of Mg-MOF-74 for CO<sub>2</sub> could be effectively increased by optimizing the amount of acetic acid. On this basis, the bimetal MOF-74 adsorbent was prepared by metal modification. The multi-component dynamic adsorption penetration analysis was utilized to examine the CO<sub>2</sub> adsorption capacity and CO<sub>2</sub>/N<sub>2</sub> selectivity of the diverse adsorbent materials. The results showed that Ni<sub>0.11</sub>/Mg<sub>0.89</sub>-MOF-74 showed a CO<sub>2</sub> adsorption capacity of 7.02 mmol/g under pure CO<sub>2</sub> atmosphere and had a selectivity of 20.50 for CO<sub>2</sub>/N<sub>2</sub> under 15% CO<sub>2</sub>/85% N<sub>2</sub> conditions, which was 10.2% and 18.02% higher than that of Mg-MOF-74 respectively. Combining XPS, SEM and N<sub>2</sub> adsorption-desorption characterization analysis, it was attributed to the effect of the more stable unsaturated metal sites Ni into the Mg-MOF-74 on the pore structure and the synergistic interaction between the two metals. Density Functional Theory (DFT) simulations revealed that the synergistic interaction between modulated the electrostatic potential strength and gradient of the material, which was more favorable for the adsorption of CO<sub>2</sub> molecules with small diameters and large quadrupole moment. In addition, the Ni<sub>0.11</sub>/Mg<sub>0.89</sub>-MOF-74 showed commendable cyclic stability, underscoring its promising potential for practical applications.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 11","pages":"Pages 1745-1758"},"PeriodicalIF":0.0,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-11-01DOI: 10.1016/S1872-5813(24)60474-3
Qi LIU , Yanqing DOU , Zhouting GONG , Shoujun LIU , Liangyu CHEN , Yuwen TAO , Jinfang LIU , Song Yang
{"title":"Research on improving carbon oxidation by fluorine doping in carbon-assisted water electrolysis for hydrogen production","authors":"Qi LIU , Yanqing DOU , Zhouting GONG , Shoujun LIU , Liangyu CHEN , Yuwen TAO , Jinfang LIU , Song Yang","doi":"10.1016/S1872-5813(24)60474-3","DOIUrl":"10.1016/S1872-5813(24)60474-3","url":null,"abstract":"<div><div>Faced with the constraints of the “carbon peaking and carbon neutrality goals”, the electrolysis of water for hydrogen production has received significant attention. However, high energy consumption is one of the problems hindering the industrialization of the technology. A strategy for “sacrificial anode carbon-assisted electrolysis of water for hydrogen production” is thus proposed, which uses the carbon oxidation reaction (COR) instead of the oxygen evolution reaction (OER) to achieve a significant reduction in energy consumption. In particular, F-doped biochar (denoted as F-BC-850) was prepared using a simple two-step carbonization method. The structural properties were analyzed using XRD, SEM-EDS, thermogravimetric, XPS and other characterization techniques. The structure-activity relationship was elucidated by electrochemical tests. The results showed that the energy consumption in 0.5 mol/L H<sub>2</sub>SO<sub>4</sub> solution at 10 mA/cm<sup>2</sup> was 57.9% of the conventional Pt sheet electrode. Characterization results showed that HF generated by the pyrolysis of ammonium fluoride etched the biochar and formed highly active C–F bonds, which improved the oxidation performance of carbon. The addition of F species changed the carbon structure, promoted the decomposition of H<sub>2</sub>O molecules to *OH radicals, and thus increased the adsorption ability of carbon atoms for *OH radicals. This work can provide theoretical guidelines for the efficient production of H<sub>2</sub> by carbon-assisted electrolysis of water and high-quality utilization of biomass.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 11","pages":"Pages 1728-1735"},"PeriodicalIF":0.0,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723038","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-11-01DOI: 10.1016/S1872-5813(24)60475-5
Jinchao HU , Tian CHANG , Mingyan XIAO , Tian ZHANG , Xue HE
{"title":"Non-thermal plasma-catalytic reforming of tar over Ni-based catalysts","authors":"Jinchao HU , Tian CHANG , Mingyan XIAO , Tian ZHANG , Xue HE","doi":"10.1016/S1872-5813(24)60475-5","DOIUrl":"10.1016/S1872-5813(24)60475-5","url":null,"abstract":"<div><div>In the process of biomass gasification to produce syngas (H<sub>2</sub>/CO), the production of tar as a by-product causes environmental pollution and hinders the development of gasification technology. The combination of non-thermal plasma and nickel-based catalysts can take advantage of the low reaction temperature of plasma and the high selectivity of catalyst to transform tar into syngas. However, carbon deposition of nickel particles in the reforming process easily causes catalyst deactivation, so designing and modifying the catalyst to improve its carbon resistance is the key to solving the catalyst deactivation problem. In this paper, the deactivation mechanism of nickel-based catalysts in the non-thermal plasma-catalytic reforming of tar system, the design and modification of catalysts to improve their carbon resistance, the types of the non-thermal plasma reactor and its tar reforming mechanism, the synergistic effects of non-thermal plasma and catalysts are reviewed. The research prospect of non-thermal plasma-catalytic reforming of tar system is also discussed. This paper provides a reference for the design and development of nickel-based catalysts in the non-thermal plasma-catalytic reforming of tar system.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 11","pages":"Pages 1563-1579"},"PeriodicalIF":0.0,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723031","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-11-01DOI: 10.1016/S1872-5813(24)60470-6
Yan YANG , Taochenxi GE , Yanan JIANG , Xian ZHANG , Yuan LIU
{"title":"In-situ growth of nickel-based catalysts on the surface of macroporous Al2O3 for CO2 methanation","authors":"Yan YANG , Taochenxi GE , Yanan JIANG , Xian ZHANG , Yuan LIU","doi":"10.1016/S1872-5813(24)60470-6","DOIUrl":"10.1016/S1872-5813(24)60470-6","url":null,"abstract":"<div><div>Macroporous catalysts often exhibit excellent mass and heat transfer properties, which can reduce pressure drop and mitigate hot spot formation during the reaction process. Addressing the issues of the active component sintering due to the strong exothermicity of CO<sub>2</sub> methanation and the demand for operation at high space velocities, in this work, a nickel-based catalyst with high surface area and large pore size and pore volume was prepared by <em>in-situ</em> growth of NiMgAl layered double hydroxide (NiMgAl-LDH) precursors on the surface of macroporous Al<sub>2</sub>O<sub>3</sub>. The effects of calcination temperature, reduction temperature, and space velocity on the catalyst structure and reaction performance were investigated. The results demonstrate that the catalyst phase composition can be controlled by adjusting the calcination temperature, while the reduction degree of Ni is regulated by altering the reduction temperature, which are effective in inhibiting the sintering of Ni, increasing the number of active Ni<sup>0</sup> sites, and then enhancing the catalytic activity of Ni-MgO/Al<sub>2</sub>O<sub>3</sub>. By conducting the calcination of NiMgAl-LDH precursor at 400 °C and subsequent reduction at 650 °C, the resulted Ni-MgO/Al<sub>2</sub>O<sub>3</sub> catalyst shows the highest active Ni surface area and exhibits the highest CO<sub>2</sub> conversion and CH<sub>4</sub> selectivity in the CO<sub>2</sub> methanation, suggesting that the surface area of metal nickel is a crucial factor for the catalytic performance of Ni-MgO/Al<sub>2</sub>O<sub>3</sub>. Furthermore, the Ni-MgO/Al<sub>2</sub>O<sub>3</sub> catalyst performs well at a high space velocity of WHSV = 80000 mL/(g·h) and a good stability at 550 °C, where the CO<sub>2</sub> conversion and CH<sub>4</sub> selectivity keep at 54% and 79%, respectively.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 11","pages":"Pages 1664-1673"},"PeriodicalIF":0.0,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142722454","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-11-01DOI: 10.1016/S1872-5813(24)60467-6
Xi TIAN , Peng YE , Qilong WU , Shangchao XIONG , Lina GAN , Jianjun CHEN
{"title":"Low-vanadium and high-activity SCR catalyst for low-temperature denitrification: Influence of vanadium precursor and surface vanadium concentration","authors":"Xi TIAN , Peng YE , Qilong WU , Shangchao XIONG , Lina GAN , Jianjun CHEN","doi":"10.1016/S1872-5813(24)60467-6","DOIUrl":"10.1016/S1872-5813(24)60467-6","url":null,"abstract":"<div><div>Nitrogen oxides (NO<sub><em>x</em></sub>), as the main pollutants of air pollution, cause serious harm to the ecological environment and human health. SCR technology is widely used as the most effective method for treating NO<sub><em>x</em></sub>. The core of SCR technology is SCR catalyst. The reaction temperature of traditional commercial catalysts is difficult to reach the optimal operating temperature range, so expanding the temperature window of V<sub>2</sub>O<sub>5</sub>/TiO<sub>2</sub> catalysts to the low-temperature region while reducing vanadium loading is a key issue to be solved. A series of V<sub>2</sub>O<sub>5</sub>/TiO<sub>2</sub> catalysts with different vanadium precursors and different vanadium loadings were prepared by solid-phase synthesis method. The physicochemical properties of the catalyst were analyzed by X-ray diffraction, X-ray photoelectron spectroscopy, temperature programmed desorption of ammonia and temperature programmed reduction of hydrogen. The denitrification activity of the catalyst was evaluated in a fixed bed reactor. The catalysts prepared with vanadyl oxalate (VOC<sub>2</sub>O<sub>4</sub>·<em>x</em>H<sub>2</sub>O) and vanadyl acetylacetonate (VO(acac)<sub>2</sub>) as vanadium precursors with a vanadium loading of 5% exhibited the highest denitrification activity, with a stable NO<sub><em>x</em></sub> conversion of 100% within the temperature range of 200–350 °. Compared with the catalysts prepared with ammonium metavanadate (NH<sub>4</sub>VO<sub>3</sub>) and vanadyl sulfate (VOSO<sub>4</sub>·<em>x</em>H<sub>2</sub>O) as the vanadium precursors, the maximum activity temperature of VOC<sub>2</sub>O<sub>4</sub>-V5Ti and VO(acac)<sub>2</sub>-V5Ti shifted towards the low-temperature region by about 150 °. Furthermore, the denitrification activity of catalyst with a low vanadium content (1%) prepared using VO(acac)<sub>2</sub> precursor was even higher than that of catalyst with a high vanadium content (6%) prepared using NH<sub>4</sub>VO<sub>3</sub> precursor. Using VOC<sub>2</sub>O<sub>4</sub> and VO(acac)<sub>2</sub> as vanadium precursors could effectively regulate the active sites and polymeric states on the catalysts, and promote the interaction of V atoms with different valence states to form more reductive V species (V<sup>4+</sup>), thus exhibiting excellent SCR reactivity. This study provided an effective method for the preparation of low-vanadium and high-activity denitrification catalysts at low temperatures.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 11","pages":"Pages 1696-1705"},"PeriodicalIF":0.0,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723036","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-10-01DOI: 10.1016/S1872-5813(24)60451-2
TANG Bowen, ZHANG Rui, LIU Haiyun, JIN Lijun, HU Haoquan
{"title":"Direct liquefaction behavior of Shenhua Shangwan coal under CO containing atmosphere","authors":"TANG Bowen, ZHANG Rui, LIU Haiyun, JIN Lijun, HU Haoquan","doi":"10.1016/S1872-5813(24)60451-2","DOIUrl":"10.1016/S1872-5813(24)60451-2","url":null,"abstract":"<div><div>Direct coal liquefaction (DCL) under CO or syngas atmosphere is beneficial to reduce the cost of hydrogen production. Effects of CO on liquefaction process of Shangwan coal were investigated by comparing the liquefaction behavior in three atmospheres of CO, H<sub>2,</sub> and N<sub>2</sub>. Then, effects of different CO/H<sub>2</sub> ratios and catalysts on the liquefaction process in syngas were investigated. The results indicated that the oil yield under CO atmosphere reached 43.1%, which was 4.2% lower than that under H<sub>2</sub>, but 10.2% higher than that under N<sub>2</sub>. The liquefaction performance was further improved by adding the Shenhua 863 catalyst. It is analyzed that CO promoted liquefaction in two ways: water-gas shift reaction and the reaction between CO and organic structures of coal. Through characterization of the products by GC-MS and FT-IR, it was found that CO makes benzenes, aliphatics, and oxygen-containing compounds in liquefied oil simultaneously increased. The effect on functional groups and free radicals concentration in the solid products was not obvious. The experimental results under syngas showed that the highest oil yield, 57.4%, can be obtained in DCL with 20% CO syngas, and further improved by increasing moisture content of coal appropriately. In addition, the Shenhua 863 catalyst had a good catalytic effect on the liquefaction process and also water-gas shift reaction.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 10","pages":"Pages 1375-1386"},"PeriodicalIF":0.0,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142532725","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-10-01DOI: 10.1016/S1872-5813(24)60460-3
WANG Yuning , GONG Jiesong , ZHOU Jiabin , CHEN Zhiyuan , TIAN Dong , NA Wei , GAO Wengui
{"title":"Mechanism of methanol synthesis from CO2 hydrogenation over Rh16/In2O3 catalysts: A combined study on density functional theory and microkinetic modeling","authors":"WANG Yuning , GONG Jiesong , ZHOU Jiabin , CHEN Zhiyuan , TIAN Dong , NA Wei , GAO Wengui","doi":"10.1016/S1872-5813(24)60460-3","DOIUrl":"10.1016/S1872-5813(24)60460-3","url":null,"abstract":"<div><div>In this study, the hydrogenation of carbon dioxide (CO<sub>2</sub>) to methanol (CH<sub>3</sub>OH) over Rh<sub>16</sub>/In<sub>2</sub>O<sub>3</sub> catalyst was studied through Density Functional Theory (DFT) and microdynamics modeling. The spontaneous dissociation mechanisms of H<sub>2</sub> and CO<sub>2</sub> adsorption at the Rh<sub>16</sub>/In<sub>2</sub>O<sub>3</sub> interface were investigated. The oxygen vacancies in In<sub>2</sub>O<sub>3</sub> enhanced the adsorption process. Bader charge analysis revealed a marginal positive charge on Rh<sub>16</sub>, elucidating the critical insights into the electronic characteristics and catalytic activity. The study established the RWGS+CO-Hydro pathway as the predominant mechanism for methanol synthesis, characterized by a sequential transformation of intermediates: CO<sub>2</sub>*→COOH*→CO*+OH*→HCO*→CH<sub>2</sub>O*→CH<sub>2</sub>OH*→CH<sub>3</sub>OH*. Furthermore, Degree of Reaction Rate Control (DRC) analysis conducted in the range of 373–873 K and 10<sup>–2</sup> to 10<sup>3</sup> bar identified two principal kinetic phenomena: at lower temperature and higher pressure, the conversion of CO* + H* to HCO* significantly impacted the overall reaction rate. Conversely, at higher temperature, the step from CH<sub>2</sub>O* + H* to CH<sub>3</sub>O* was dominate.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 10","pages":"Pages 1462-1473"},"PeriodicalIF":0.0,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142532726","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
燃料化学学报Pub Date : 2024-10-01DOI: 10.1016/S1872-5813(24)60459-7
HUANG Min , BO Qifei , LI Juan , QIAO Jingxuan , YUAN Shanliang , ZHANG Biao , CHEN Honglin , JIANG Yi
{"title":"Hydrogen production via steam reforming of methanol on Cu/ZnO/Al2O3 catalysts: Effects of Al2O3 precursors","authors":"HUANG Min , BO Qifei , LI Juan , QIAO Jingxuan , YUAN Shanliang , ZHANG Biao , CHEN Honglin , JIANG Yi","doi":"10.1016/S1872-5813(24)60459-7","DOIUrl":"10.1016/S1872-5813(24)60459-7","url":null,"abstract":"<div><div>A series of Cu/ZnO/Al<sub>2</sub>O<sub>3</sub> catalysts were prepared by co-precipitation method. This research focuses on investigating the influence of different Al<sub>2</sub>O<sub>3</sub> precursors on the catalyst structure through thorough structural characterization techniques. Additionally, the catalytic performance of these catalysts in methanol reforming for hydrogen production was systematically evaluated. The results indicate that the simultaneous co-precipitation of Al<sup>3+</sup> with Cu<sup>2+</sup> and Zn<sup>2+</sup> leads to partial substitution of Cu-Zn in the basic carbonates by Al<sup>3+</sup>. This substitution forms a hydrotalcite-like structure and strengthens Zn-Al interactions. On the contrary, after the co-precipitation of Cu<sup>2+</sup> and Zn<sup>2+</sup>, introducing the Al<sub>2</sub>O<sub>3</sub> precursor has a positive effect on eliminating the adverse effects of Al<sup>3+</sup> on Cu-Zn substitution in basic carbonates. This process promotes the Cu-ZnO interaction, facilitates the dispersion of CuO species, and enhances the reducibility of catalysts. It also improves the dispersion of Cu on the surface, and ultimately enhanced the catalytic activity. Notably, the catalyst prepared using pseudo-boehmite as the Al<sub>2</sub>O<sub>3</sub> precursor exhibited the highest activity. Under the conditions of a H<sub>2</sub>O/CH<sub>3</sub>OH molar ratio of 1.2 and a reaction temperature of 493 K, methanol conversion reached 94.8%, and the H<sub>2</sub> space-time yield was 97.5 mol/(kg·h). The catalyst activity remained relatively stable after continuous operation for 25 h. Even after being heat-treated at 723 K for 10 h, the activity loss of the catalyst was only 5.37%.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"52 10","pages":"Pages 1443-1453"},"PeriodicalIF":0.0,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142532728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}