燃料化学学报最新文献

Effect of heat treatment on the performance of ZnOHF for electrocatalytic reduction of CO2 to CO

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60485-8

Shuling CHANG , Tingting SUN , Rongjing JIA , Lihong ZHANG , Yanhong XU

The selective and efficient conversion of inert CO₂ into value-added chemicals by electrochemical methods is one of the important ways to alleviate the environmental and energy crisis. Non-precious metal Zn is often used in the electrocatalytic reduction reaction of CO₂ (CO₂RR) to CO due to its abundant reserves, low price, good stability and non-toxic. However, it is still necessary to improve the catalytic performance of traditional Zn-based catalysts for CO₂RR. In order to optimize the performance of Zn-based catalysts, pure ZnOHF sample was synthesized by hydrothermal method. The effect of heat treatment on the structure, texture and electrocatalytic CO₂RR performance of the samples was investigated. The electrocatalytic evaluation results revealed that the heat-treated ZnOHF sample showed better activity and CO selectivity compared with untreated sample. The Faraday efficiency of CO (FE_CO) reached 77.4% at −1.15V vs. RHE. Even at potential of −1.05 V vs. RHE, the current density and FE_CO could be stabilized at −6.17 mA/cm² and 72% in 5 h. This was because heat treatment optimized the amount of surface hydroxyl of ZnOHF. The microcrystalline particles became uniform and fine. The roughness and electrochemical surface area (ECSA) also increased, thus exposing more active sites and promoting the adsorption and activation of CO₂ as well as the desorption of CO. This study provides experimental basis and theoretical guidance for the design and development of Zn-based catalysts for electrocatalytic CO₂RR.

{"title":"Effect of heat treatment on the performance of ZnOHF for electrocatalytic reduction of CO2 to CO","authors":"Shuling CHANG , Tingting SUN , Rongjing JIA , Lihong ZHANG , Yanhong XU","doi":"10.1016/S1872-5813(24)60485-8","DOIUrl":"10.1016/S1872-5813(24)60485-8","url":null,"abstract":"<div><div>The selective and efficient conversion of inert CO<sub>2</sub> into value-added chemicals by electrochemical methods is one of the important ways to alleviate the environmental and energy crisis. Non-precious metal Zn is often used in the electrocatalytic reduction reaction of CO<sub>2</sub> (CO<sub>2</sub>RR) to CO due to its abundant reserves, low price, good stability and non-toxic. However, it is still necessary to improve the catalytic performance of traditional Zn-based catalysts for CO<sub>2</sub>RR. In order to optimize the performance of Zn-based catalysts, pure ZnOHF sample was synthesized by hydrothermal method. The effect of heat treatment on the structure, texture and electrocatalytic CO<sub>2</sub>RR performance of the samples was investigated. The electrocatalytic evaluation results revealed that the heat-treated ZnOHF sample showed better activity and CO selectivity compared with untreated sample. The Faraday efficiency of CO (FE<sub>CO</sub>) reached 77.4% at −1.15V <em>vs.</em> RHE. Even at potential of −1.05 V <em>vs.</em> RHE, the current density and FE<sub>CO</sub> could be stabilized at −6.17 mA/cm<sup>2</sup> and 72% in 5 h. This was because heat treatment optimized the amount of surface hydroxyl of ZnOHF. The microcrystalline particles became uniform and fine. The roughness and electrochemical surface area (ECSA) also increased, thus exposing more active sites and promoting the adsorption and activation of CO<sub>2</sub> as well as the desorption of CO. This study provides experimental basis and theoretical guidance for the design and development of Zn-based catalysts for electrocatalytic CO<sub>2</sub>RR.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 4","pages":"Pages 452-461"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858896","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}

引用次数: 0

Preparation CuxCo1–x for photocatalytic conversion of CO2

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60506-2

Jingzhou WANG, Chenzhong YAO, Xisheng ZHANG, Ziwei MA

Metal nanoparticles with high surface area and high electrochemical activity exhibit excellent catalytic performance in the photocatalytic reduction of carbon dioxide (CO₂). However, poor stability, small specific surface area, and less active sites limits its solar energy utilization. Hydrothermal method was utilized to synthesize the bimetallic material of Cu_xCo_1−x in this work. Co was loaded onto the Cu surface due to the electrons generated by the surface plasmon resonance (SPR) effect occurring on the Cu surface. Cu_xCo_1−x exhibits high photocatalytic conversion of CO₂ efficiency under irradiation, which mainly because the Co nanoparticles on the surface of Cu can be used as cocatalysts to enhance the photocharge transfer. Cu_0.6Co_0.4 exhibits the comparatively best photocatalytic conversion efficiency of CO₂ in the first 6 h light irradiation. The yields of CO and CH₄ reached 35.26 and 2.71 μmol/(g·h), respectively. Upon illumination, electrons were produced, with the majority of them moving towards the interface. This movement contributes to the increased lifetime of photogenerated electron-hole pairs, which in turn boosts the photocatalytic efficiency. The findings of this research provide significant insights for creating photocatalysts that are both highly effective and stable in CO₂ reduction processes.

{"title":"Preparation CuxCo1–x for photocatalytic conversion of CO2","authors":"Jingzhou WANG, Chenzhong YAO, Xisheng ZHANG, Ziwei MA","doi":"10.1016/S1872-5813(24)60506-2","DOIUrl":"10.1016/S1872-5813(24)60506-2","url":null,"abstract":"<div><div>Metal nanoparticles with high surface area and high electrochemical activity exhibit excellent catalytic performance in the photocatalytic reduction of carbon dioxide (CO<sub>2</sub>). However, poor stability, small specific surface area, and less active sites limits its solar energy utilization. Hydrothermal method was utilized to synthesize the bimetallic material of Cu<sub><em>x</em></sub>Co<sub>1−<em>x</em></sub> in this work. Co was loaded onto the Cu surface due to the electrons generated by the surface plasmon resonance (SPR) effect occurring on the Cu surface. Cu<sub><em>x</em></sub>Co<sub>1−<em>x</em></sub> exhibits high photocatalytic conversion of CO<sub>2</sub> efficiency under irradiation, which mainly because the Co nanoparticles on the surface of Cu can be used as cocatalysts to enhance the photocharge transfer. Cu<sub>0.6</sub>Co<sub>0.4</sub> exhibits the comparatively best photocatalytic conversion efficiency of CO<sub>2</sub> in the first 6 h light irradiation. The yields of CO and CH<sub>4</sub> reached 35.26 and 2.71 μmol/(g·h), respectively. Upon illumination, electrons were produced, with the majority of them moving towards the interface. This movement contributes to the increased lifetime of photogenerated electron-hole pairs, which in turn boosts the photocatalytic efficiency. The findings of this research provide significant insights for creating photocatalysts that are both highly effective and stable in CO<sub>2</sub> reduction processes.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 4","pages":"Pages 462-471"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858897","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}

引用次数: 0

Research progress on metal-support interactions over Ni-based catalysts for CH4-CO2 reforming reaction

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60500-1

Kai SUN, Jianfei JIANG, Zixuan LIU, Shiqi GENG, Zhenmin LIU, Jiaqian YANG, Shasha LI

With ongoing global warming and increasing energy demands, the CH₄-CO₂ reforming reaction (dry reforming of methane, DRM) has garnered significant attention as a promising carbon capture and utilization technology. Nickel-based catalysts are renowned for their outstanding activity and selectivity in this process. The impact of metal-support interaction (MSI), on Ni-based catalyst performance has been extensively researched and debated recently. This paper reviews the recent research progress of MSI on Ni-based catalysts and their characterization and modulation strategies in catalytic reactions. From the perspective of MSI, the effects of different carriers (metal oxides, carbon materials and molecular sieves, etc.) are introduced on the dispersion and surface structure of Ni active metal particles, and the effect of MSI on the activity and stability of DRM reactions on Ni-based catalysts is discussed in detail. Future research should focus on better understanding and controlling MSI to improve the performance and durability of nickel-based catalysts in CH₄-CO₂ reforming, advancing cleaner energy technologies.

{"title":"Research progress on metal-support interactions over Ni-based catalysts for CH4-CO2 reforming reaction","authors":"Kai SUN, Jianfei JIANG, Zixuan LIU, Shiqi GENG, Zhenmin LIU, Jiaqian YANG, Shasha LI","doi":"10.1016/S1872-5813(24)60500-1","DOIUrl":"10.1016/S1872-5813(24)60500-1","url":null,"abstract":"<div><div>With ongoing global warming and increasing energy demands, the CH<sub>4</sub>-CO<sub>2</sub> reforming reaction (dry reforming of methane, DRM) has garnered significant attention as a promising carbon capture and utilization technology. Nickel-based catalysts are renowned for their outstanding activity and selectivity in this process. The impact of metal-support interaction (MSI), on Ni-based catalyst performance has been extensively researched and debated recently. This paper reviews the recent research progress of MSI on Ni-based catalysts and their characterization and modulation strategies in catalytic reactions. From the perspective of MSI, the effects of different carriers (metal oxides, carbon materials and molecular sieves, etc.) are introduced on the dispersion and surface structure of Ni active metal particles, and the effect of MSI on the activity and stability of DRM reactions on Ni-based catalysts is discussed in detail. Future research should focus on better understanding and controlling MSI to improve the performance and durability of nickel-based catalysts in CH<sub>4</sub>-CO<sub>2</sub> reforming, advancing cleaner energy technologies.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 4","pages":"Pages 434-451"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858966","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}

引用次数: 0

A review of research on perovskite oxygen carrier for chemical looping reforming of methane

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60498-6

Jinli REN , Genning ZHANG , Qiuwan SHEN , Xinhai LI , Yanqiu DU , Binjian CHEN , Min YAN

The chemical looping reforming of methane can simultaneously produce synthesis gas and high-purity hydrogen, and efficiently capture CO₂ during the hydrogen production process, which is of great significance for achieving the “dual carbon” goal. The selection of high-performance and low-cost oxygen carriers is crucial for the chemical looping reforming of methane. Due to its abundant oxygen vacancies and good thermal stability, the perovskite oxygen carriers have become a research hotspot as the oxygen carriers required for the chemical looping reforming of methane. In this review, the chemical looping reforming of methane including chemical looping steam methane reforming, chemical looping dry reforming of methane and chemical looping partial oxidation reforming of methane was first introduced. Then, the latest research progress on the Fe based, Ni based and Mn based perovskite type oxygen carriers as well as the supported perovskite oxygen carriers was summarized. Moreover, the pore structure, surface morphology, redox performance, and reaction mechanism of different metal-based perovskite oxygen carriers were analyzed and compared. Finally, the challenges and development prospects faced by perovskite oxygen carriers were summarized.

{"title":"A review of research on perovskite oxygen carrier for chemical looping reforming of methane","authors":"Jinli REN , Genning ZHANG , Qiuwan SHEN , Xinhai LI , Yanqiu DU , Binjian CHEN , Min YAN","doi":"10.1016/S1872-5813(24)60498-6","DOIUrl":"10.1016/S1872-5813(24)60498-6","url":null,"abstract":"<div><div>The chemical looping reforming of methane can simultaneously produce synthesis gas and high-purity hydrogen, and efficiently capture CO<sub>2</sub> during the hydrogen production process, which is of great significance for achieving the “dual carbon” goal. The selection of high-performance and low-cost oxygen carriers is crucial for the chemical looping reforming of methane. Due to its abundant oxygen vacancies and good thermal stability, the perovskite oxygen carriers have become a research hotspot as the oxygen carriers required for the chemical looping reforming of methane. In this review, the chemical looping reforming of methane including chemical looping steam methane reforming, chemical looping dry reforming of methane and chemical looping partial oxidation reforming of methane was first introduced. Then, the latest research progress on the Fe based, Ni based and Mn based perovskite type oxygen carriers as well as the supported perovskite oxygen carriers was summarized. Moreover, the pore structure, surface morphology, redox performance, and reaction mechanism of different metal-based perovskite oxygen carriers were analyzed and compared. Finally, the challenges and development prospects faced by perovskite oxygen carriers were summarized.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 4","pages":"Pages 419-433"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858895","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}

引用次数: 0

Preparation of Fe/SAPO-34 catalyst and its performance in CO hydrogenation to light olefins

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60505-0

Liuliu LI , Mingwei ZHANG , Yingjun WANG , Kegong FANG

Fischer-Tropsch synthesis is an important route to synthesize light olefins from syngas. However, precise control of the product selectivity and enhancing carbon utilization efficiency remains a challenge. Herein, a series of Fe/SAPO-34 catalysts with different Fe contents were prepared using negative pressure impregnation method, and their performance in CO hydrogenation reaction was evaluated. Combined N₂ adsorption/desorption, XRD, SEM, NH₃-TPD, and CO-TPD characterizations, the structure-performance relationship of the Fe/SAPO-34 catalysts was clarified. The results showed that with the increase of Fe loading, the strength and quantity of the acidity of the catalysts decreased sequentially, while the CO non-dissociation activation ability was weakened and the CO dissociation activation ability was enhanced, resulting in an increasing and decreasing trend in the selectivity of light olefins and oxygenates, respectively. Under a mild reaction conditions of t=200°C, p=2.0 MPa, GHSV=3300 h^–1, in the carbon products containing CO₂, the selectivity of light olefins and oxygenates over 5%Fe/SAPO-34 catalyst was 16.2% and 52.6%, respectively; while that over 25%Fe/SAPO-34 catalyst was 31.9% and 16.9%, respectively. A reasonable reaction mechanism was proposed based on the in situ IR characterization. This study provides a new way for the research and development of catalyst for light olefins synthesis with enhanced carbon utilization efficiency, showing promising application prospects.

{"title":"Preparation of Fe/SAPO-34 catalyst and its performance in CO hydrogenation to light olefins","authors":"Liuliu LI , Mingwei ZHANG , Yingjun WANG , Kegong FANG","doi":"10.1016/S1872-5813(24)60505-0","DOIUrl":"10.1016/S1872-5813(24)60505-0","url":null,"abstract":"<div><div>Fischer-Tropsch synthesis is an important route to synthesize light olefins from syngas. However, precise control of the product selectivity and enhancing carbon utilization efficiency remains a challenge. Herein, a series of Fe/SAPO-34 catalysts with different Fe contents were prepared using negative pressure impregnation method, and their performance in CO hydrogenation reaction was evaluated. Combined N<sub>2</sub> adsorption/desorption, XRD, SEM, NH<sub>3</sub>-TPD, and CO-TPD characterizations, the structure-performance relationship of the Fe/SAPO-34 catalysts was clarified. The results showed that with the increase of Fe loading, the strength and quantity of the acidity of the catalysts decreased sequentially, while the CO non-dissociation activation ability was weakened and the CO dissociation activation ability was enhanced, resulting in an increasing and decreasing trend in the selectivity of light olefins and oxygenates, respectively. Under a mild reaction conditions of <em>t</em>=200°C, <em>p</em>=2.0 MPa, GHSV=3300 h<sup>–1</sup>, in the carbon products containing CO<sub>2</sub>, the selectivity of light olefins and oxygenates over 5%Fe/SAPO-34 catalyst was 16.2% and 52.6%, respectively; while that over 25%Fe/SAPO-34 catalyst was 31.9% and 16.9%, respectively. A reasonable reaction mechanism was proposed based on the <em>in situ</em> IR characterization. This study provides a new way for the research and development of catalyst for light olefins synthesis with enhanced carbon utilization efficiency, showing promising application prospects.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 4","pages":"Pages 504-514"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858898","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}

引用次数: 0

Synthesis of SAPO-35 molecular sieves with different structure-directing agents and their catalytic performance in the conversion of methanol to olefins

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60488-3

Ni LIANG, Lei KANG, Yujia WANG, Haiyan WANG, Yingzhi BAI, Qiao HAN, Na SUN

A series of SAPO-35 molecular sieves with different SiO₂/Al₂O₃ ratios were synthesized by hydrothermal method using hexamethylene imine (HMI) and N-methylpiperidine (NMP) as the structure-directing agent (SDA). The synthesized SAPO-35 molecular sieves were characterized by XRD, SEM, FT-IR, NH₃-TPD, XRF and N₂ sorption and their catalytic performance in the conversion of methanol to olefins (MTO) was comparatively investigated. The results indicated that the crystallinity and acid density of the SAPO-35 molecular sieves increase first and then decrease with the increase of the SiO₂/Al₂O₃ ratio in the initial gel; in particular, the SAPO-35-0.3(HMI) sample with a SiO₂/Al₂O₃ ratio of 0.3 displays a high crystallinity, large surface area and suitable acid distribution as a catalyst in MTO. Compared with the SAPO-35-HMI sample synthesized with HMI as SDA, the SAPO-35-NMP sample having the same SiO₂/Al₂O₃ ratio but synthesized using new NMP as SDA exhibits much better catalytic stability and higher selectivity to light olefins in MTO; the selectivity to ethene + propene reaches 81.3%, where ethene accounts for more than 50%, far surpassing propene.

{"title":"Synthesis of SAPO-35 molecular sieves with different structure-directing agents and their catalytic performance in the conversion of methanol to olefins","authors":"Ni LIANG, Lei KANG, Yujia WANG, Haiyan WANG, Yingzhi BAI, Qiao HAN, Na SUN","doi":"10.1016/S1872-5813(24)60488-3","DOIUrl":"10.1016/S1872-5813(24)60488-3","url":null,"abstract":"<div><div>A series of SAPO-35 molecular sieves with different SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratios were synthesized by hydrothermal method using hexamethylene imine (HMI) and <em>N</em>-methylpiperidine (NMP) as the structure-directing agent (SDA). The synthesized SAPO-35 molecular sieves were characterized by XRD, SEM, FT-IR, NH<sub>3</sub>-TPD, XRF and N<sub>2</sub> sorption and their catalytic performance in the conversion of methanol to olefins (MTO) was comparatively investigated. The results indicated that the crystallinity and acid density of the SAPO-35 molecular sieves increase first and then decrease with the increase of the SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratio in the initial gel; in particular, the SAPO-35-0.3(HMI) sample with a SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratio of 0.3 displays a high crystallinity, large surface area and suitable acid distribution as a catalyst in MTO. Compared with the SAPO-35-HMI sample synthesized with HMI as SDA, the SAPO-35-NMP sample having the same SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratio but synthesized using new NMP as SDA exhibits much better catalytic stability and higher selectivity to light olefins in MTO; the selectivity to ethene + propene reaches 81.3%, where ethene accounts for more than 50%, far surpassing propene.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 4","pages":"Pages 515-526"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858899","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}

引用次数: 0

Raney Ni as a high-performance catalyst for the hydrolysis of ammonia borane to produce hydrogen

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60492-5

Tianxuan YANG, Meixia WU, Junli WANG, Ning CHEN, Changqiang TANG, Jiang LI, Jianpeng SHANG, Yong GUO, Zuopeng LI

Ammonia borane (AB) has received much attention as an environmentally friendly, non-toxic, room temperature stable hydrogen storage material with high hydrogen content of 19.6%. However, its hydrolysis for hydrogen production at room-temperature is kinetically slow and requires precious metal catalysts. In this work, it is found that the prepared Raney Ni W-r treated with high concentration of NaOH (6.25 mol/L) at 110 °C exhibited excellent catalytic performance for AB hydrolysis at room temperature. The Raney Ni W-r can promote the AB complete hydrolysis within 60 s under basic condition at small sized trials, even higher than that of the 20% Pt/C catalyst. Its apparent activation energy at room temperature is only 26.6 kJ/mol and the turnover frequency (TOF) value is as high as 51.42 min⁻¹. Owing to its high density and magnetic properties, the catalyst is very easy for magnetic separation. Furthermore, possible mechanism of the hydrolytic reaction of AB based on experimental results is proposed. As a well-established industrial catalyst, Raney Ni has been prepared on a large scale at low cost. This study provides a promising pathway for the large-scale preparation of low-cost and recyclable catalysts for AB hydrolysis.

{"title":"Raney Ni as a high-performance catalyst for the hydrolysis of ammonia borane to produce hydrogen","authors":"Tianxuan YANG, Meixia WU, Junli WANG, Ning CHEN, Changqiang TANG, Jiang LI, Jianpeng SHANG, Yong GUO, Zuopeng LI","doi":"10.1016/S1872-5813(24)60492-5","DOIUrl":"10.1016/S1872-5813(24)60492-5","url":null,"abstract":"<div><div>Ammonia borane (AB) has received much attention as an environmentally friendly, non-toxic, room temperature stable hydrogen storage material with high hydrogen content of 19.6%. However, its hydrolysis for hydrogen production at room-temperature is kinetically slow and requires precious metal catalysts. In this work, it is found that the prepared Raney Ni W-r treated with high concentration of NaOH (6.25 mol/L) at 110 °C exhibited excellent catalytic performance for AB hydrolysis at room temperature. The Raney Ni W-r can promote the AB complete hydrolysis within 60 s under basic condition at small sized trials, even higher than that of the 20% Pt/C catalyst. Its apparent activation energy at room temperature is only 26.6 kJ/mol and the turnover frequency (TOF) value is as high as 51.42 min<sup>−1</sup>. Owing to its high density and magnetic properties, the catalyst is very easy for magnetic separation. Furthermore, possible mechanism of the hydrolytic reaction of AB based on experimental results is proposed. As a well-established industrial catalyst, Raney Ni has been prepared on a large scale at low cost. This study provides a promising pathway for the large-scale preparation of low-cost and recyclable catalysts for AB hydrolysis.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 4","pages":"Pages 555-564"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858900","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}

引用次数: 0

Preparation and hydrogen storage properties of metal-organic framework UiO-66: Comparison of microwave and conventional hydrothermal preparation

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60496-2

Ruiqi Wang , Hengjie Shi , Yanli Sun , Xi Zhang , Caizhu Liu , Yuhua Wu , Jianbo Wu , Hui Zhang , Hongcun Bai

The efficient preparation of metal-organic frameworks (MOFs) has become an important issue in the field of solid-state hydrogen storage due to the advantages of strong structural design and tunable pores of MOFs. However, its efficient preparation is still facing key bottlenecks such as process complexity, long cycle time and low efficiency. Microwave-assisted synthesis is an emerging technology that utilizes microwave external fields to enhance the mass and heat transfer and reaction behavior during the preparation of porous materials, thus promising to improve the preparation efficiency of MOFs materials. This method is considered to be an important development to realize the efficient preparation of MOFs materials. This work focuses on the comparative study of microwave and conventional solvothermal preparation of UiO-66 materials for efficient hydrogen storage. UiO-66 with different structures and morphologies were prepared by adjusting the crystallization temperature and crystallization time. The preparation process of UiO-66 by microwave method was optimized to obtain the optimal preparation conditions of 120 °C, 1.0 h, and its specific surface area of 1561 m²/g. In order to gain a deeper understanding of the hydrogen storage properties of the material, we have established an effective correlation between the microstructure of UiO-66 and its hydrogen storage properties. The experimental results showed that the hydrogen adsorption of the prepared UiO-66 reached 3.78% at 77 K and 5 MPa. In addition, quasi-primary and quasi-secondary kinetic equations and intra-particle diffusion models were used to quantitatively describe the kinetic laws and mechanisms of the hydrogen adsorption process of UiO-66. The research related to hydrogen storage in UiO-66 materials in this thesis provides theoretical basis and technical support for the efficient preparation and hydrogen storage mechanism of MOFs materials, and provides a reference for the application of solid-state hydrogen storage in porous materials.

由于金属有机框架（MOFs）具有结构设计性强、孔隙可调等优点，其高效制备已成为固态储氢领域的重要课题。然而，其高效制备仍面临工艺复杂、周期长、效率低等关键瓶颈。微波辅助合成是一种新兴技术，它利用微波外场来增强多孔材料制备过程中的传质、传热和反应行为，从而有望提高 MOFs 材料的制备效率。该方法被认为是实现 MOFs 材料高效制备的重要发展方向。本研究主要对微波和传统溶热制备 UiO-66 材料用于高效储氢进行了比较研究。通过调节结晶温度和结晶时间，制备了不同结构和形态的 UiO-66。对微波法制备 UiO-66 的工艺进行了优化，获得了 120 ℃、1.0 h 的最佳制备条件，其比表面积为 1561 m2/g。为了深入了解该材料的储氢性能，我们建立了 UiO-66 的微观结构与其储氢性能之间的有效关联。实验结果表明，在 77 K 和 5 MPa 条件下，制备的 UiO-66 的吸氢率达到 3.78%。此外，还利用准一级、准二级动力学方程和颗粒内扩散模型定量描述了 UiO-66 吸氢过程的动力学规律和机理。本论文对UiO-66材料储氢的相关研究为MOFs材料的高效制备和储氢机理提供了理论依据和技术支持，为多孔材料固态储氢的应用提供了参考。

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引用次数: 0

Preparation and coking property of binder pitch: Effects of modification methods

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60497-4

Yuan Qi, Chunyang Zhang, Lixin Feng, Yaming Zhu, Junxia Cheng, Xuefei Zhao

Binder pitch is a crucial raw material for producing carbon/graphite electrodes and lithium-ion battery anodes. The quality and application of carbon/graphite products largely depend on properties of the binder pitch. High-quality binder pitch plays a key role in enhancing quality of the carbon/graphite materials. In this work, refined medium pitch was used as the raw material. Effect of various modification methods on properties of the binder pitch was examined, such as molecular structure, thermal stability, and optical microstructure, along with its coking properties including optical microstructure of pitch coke, carbon microcrystalline structure, and carbon surface morphology. The results indicate that a high-quality isotropic binder pitch (softening point: 144 °C, QI content: 0.46%, TI content: 26.74%, coking value: 51.53%, volatile matter: 56.65%) was achieved using a two-step oxidation polymerization and mild thermal polymerization method. In the first step, the refined pitch was oxidized at 280 °C for 3 h; in the second, it was rapidly heated to 360 °C and held for 1 h under nitrogen atmosphere. This process produced a binder pitch with a high degree of aromatic condensation and fewer small-molecule branched structures. Optical microstructure of the binder pitch coke, produced through thermal conversion and carbonization, comprised 83.92% leaflet and fibrous structures. Degree of disorder in the binder pitch coke was relatively low, resulting in a regular and orderly microcrystalline structure. The content of carbon microcrystals exhibited a high degree of regularity, reaching 90.89%, while the ideal graphite microcrystal content I_G/I_All was 18%.

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引用次数: 0

Thermal depolymerization of polyethylene terephthalate waste and its use in coal-blending coking

Q3 Energy

燃料化学学报

Pub Date : 2025-04-01 DOI: 10.1016/S1872-5813(24)60504-9

Shixian FANG, Huan SONG, Xiangchun LIU, Ping CUI

This work proposed a strategy to improve the caking index of polyethylene terephthalate (PET) waste, in which low-temperature pyrolysis treatment (LTPT) was used to depolymerize PET waste. The mechanism of G modification was revealed combining thermogravimetric (TG) analysis, Fourier transform infrared spectroscopy, pyrolysis-gas chromatography with mass spectrometric detection, and solid-state ¹³C nuclear magnetic resonance spectroscopy. Furthermore, crucible coking experiments were also conducted using industrial coal mixture and treated PET with the optimum G (PET300) or raw PET to evaluate the applicability of PET waste in coal-blending coking. According to characterization results of coke reactivity (CR), coke strength after reaction (CSR) indices, TG-related curves, pore volumes, and Raman spectra of the resultant cokes, LTPT could greatly increase the G of PET, and the optimum temperature was 300 °C. Specifically, compared with the coke obtained from the blend with PET, the CR of the coke produced from the blend with PET300 decreased by 4.9%, whereas the CSR of the increased by 7.4%, suggesting that LTPT could increase the proportion of PET used for coal-blending coking. The improvement in G is attributed to the changes in C‒O/C=O ratio, aliphatic H and aromaticity caused by LTPT.

{"title":"Thermal depolymerization of polyethylene terephthalate waste and its use in coal-blending coking","authors":"Shixian FANG, Huan SONG, Xiangchun LIU, Ping CUI","doi":"10.1016/S1872-5813(24)60504-9","DOIUrl":"10.1016/S1872-5813(24)60504-9","url":null,"abstract":"<div><div>This work proposed a strategy to improve the caking index of polyethylene terephthalate (PET) waste, in which low-temperature pyrolysis treatment (LTPT) was used to depolymerize PET waste. The mechanism of <em>G</em> modification was revealed combining thermogravimetric (TG) analysis, Fourier transform infrared spectroscopy, pyrolysis-gas chromatography with mass spectrometric detection, and solid-state <sup>13</sup>C nuclear magnetic resonance spectroscopy. Furthermore, crucible coking experiments were also conducted using industrial coal mixture and treated PET with the optimum <em>G</em> (PET300) or raw PET to evaluate the applicability of PET waste in coal-blending coking. According to characterization results of coke reactivity (CR), coke strength after reaction (CSR) indices, TG-related curves, pore volumes, and Raman spectra of the resultant cokes, LTPT could greatly increase the <em>G</em> of PET, and the optimum temperature was 300 °C. Specifically, compared with the coke obtained from the blend with PET, the CR of the coke produced from the blend with PET300 decreased by 4.9%, whereas the CSR of the increased by 7.4%, suggesting that LTPT could increase the proportion of PET used for coal-blending coking. The improvement in <em>G</em> is attributed to the changes in C‒O/C=O ratio, aliphatic H and aromaticity caused by LTPT.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 4","pages":"Pages 602-612"},"PeriodicalIF":0.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858970","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}

引用次数: 0