Pub Date : 2025-08-01DOI: 10.1016/S1872-5813(25)60543-3
Linyao HUANG , Mi LUO , Tianhua YANG , Chenguang WANG
In this paper, a series of Cr-doped RuO2@NC catalysts (Cr0.1-RuO2@NC, Cr0.2-RuO2@NC, Cr0.4-RuO2@NC) with controlled Cr doping (0.5%, 1%, 3%) were prepared to investigate the mechanistic interplay between transition metal doping, oxygen vacancy (OV) formation and oxygen evolution reaction (OER) performance. Systematic characterization results reveal that the oxygen vacancy concentration follows a volcano-type trend with increasing Cr content, peaking at 1% Cr doping (Cr0.2-RuO2@NC). Combined X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses confirm that Cr doping effectively induces electronic structure reconstruction of RuO2, generating high-density oxygen vacancies that serve as electrochemically active sites. The optimized Cr0.2-RuO2@NC catalyst exhibits exceptional OER performance, achieving a low overpotential of 223 mV at 10 mA/cm2 and a Tafel slope of 63.8 mV/dec, significantly surpassing its 0.5% and 3% doped counterparts. Remarkably, it retains 99.9% of the initial activity after 27 h. Cr doping not only regulates the concentration of oxygen vacancies through lattice distortion. The strong Cr–O covalent bonding enhances the structural stability of the catalyst. This work establishes a general transition metal doping strategy for precise oxygen vacancy engineering, providing new design principles and theoretical foundations for developing high-performance OER electrocatalysts.
{"title":"Tuning oxygen vacancy via transition metal doping for efficient oxygen evolution reaction","authors":"Linyao HUANG , Mi LUO , Tianhua YANG , Chenguang WANG","doi":"10.1016/S1872-5813(25)60543-3","DOIUrl":"10.1016/S1872-5813(25)60543-3","url":null,"abstract":"<div><div>In this paper, a series of Cr-doped RuO<sub>2</sub>@NC catalysts (Cr<sub>0.1</sub>-RuO<sub>2</sub>@NC, Cr<sub>0.2</sub>-RuO<sub>2</sub>@NC, Cr<sub>0.4</sub>-RuO<sub>2</sub>@NC) with controlled Cr doping (0.5%, 1%, 3%) were prepared to investigate the mechanistic interplay between transition metal doping, oxygen vacancy (O<sub>V</sub>) formation and oxygen evolution reaction (OER) performance. Systematic characterization results reveal that the oxygen vacancy concentration follows a volcano-type trend with increasing Cr content, peaking at 1% Cr doping (Cr<sub>0.2</sub>-RuO<sub>2</sub>@NC). Combined X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses confirm that Cr doping effectively induces electronic structure reconstruction of RuO<sub>2</sub>, generating high-density oxygen vacancies that serve as electrochemically active sites. The optimized Cr<sub>0.2</sub>-RuO<sub>2</sub>@NC catalyst exhibits exceptional OER performance, achieving a low overpotential of 223 mV at 10 mA/cm<sup>2</sup> and a Tafel slope of 63.8 mV/dec, significantly surpassing its 0.5% and 3% doped counterparts. Remarkably, it retains 99.9% of the initial activity after 27 h. Cr doping not only regulates the concentration of oxygen vacancies through lattice distortion. The strong Cr–O covalent bonding enhances the structural stability of the catalyst. This work establishes a general transition metal doping strategy for precise oxygen vacancy engineering, providing new design principles and theoretical foundations for developing high-performance OER electrocatalysts.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 8","pages":"Pages 1173-1182"},"PeriodicalIF":0.0,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144886577","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}
Pub Date : 2025-08-01DOI: 10.1016/S1872-5813(25)60534-2
Yan CHEN, Huanhuan HE, Yufeng LI, Bing LIU, Xiaohao LIU
In Fischer-Tropsch synthesis (FTS), iron-based catalysts are prone to deactivation due to carbon deposition. To address this challenge, we developed a simple physical powder-mixing strategy by mechanically mixing iron-based FTS catalysts with oxides such as SiO2, MgO, ZnO, ZrO2, MnO2, Al2O3, and graphene oxide (GO). Experimental results demonstrate that oxide incorporation significantly suppresses carbon deposition in a composition-dependent manner, thereby enhancing catalytic stability. Notably, after mixing with SiO2 or MgO powder, the CO conversion reached 96.6% and 97.6%, respectively, maintaining stability for more than 20 h. In contrast, catalyst mixed with quartz sand particles underwent rapid deactivation within 20, with a decrease in CO conversion from 93.0% to 14.6%, accompanied by a sharp rise in CH4 selectivity. By combining various characterization methods such as XRD, Mossbauer spectroscopy, TGA, XPS and CO-TPD, the promoting mechanism of oxides on reaction stability was deeply studied. The results indicate that the catalyst mixed SiO2 powder reduced the content of active χ-Fe5C2 phases from 97% to 52.1% and effectively suppressed carbon deposition. This enhancement is attributed to the strong interfacial interactions between SiO2 and the iron-based catalyst, which moderately inhibited CO adsorption and dissociation kinetics, decelerated carbonization, and prevented rapid accumulation of carbon species on the catalyst surface. Similar mechanisms were observed over MgO additives, further validating the role of oxide-iron interactions. This work elucidates the mechanism of the interaction between iron-based catalysts and mixed oxides on carbon deposition behavior in Fischer-Tropsch synthesis reactions, providing an innovative strategy and theoretical foundation for designing highly active and stable catalysts.
{"title":"Study on the regulation of Fischer-Tropsch synthesis catalytic performance by mixing oxides with iron-based catalysts","authors":"Yan CHEN, Huanhuan HE, Yufeng LI, Bing LIU, Xiaohao LIU","doi":"10.1016/S1872-5813(25)60534-2","DOIUrl":"10.1016/S1872-5813(25)60534-2","url":null,"abstract":"<div><div>In Fischer-Tropsch synthesis (FTS), iron-based catalysts are prone to deactivation due to carbon deposition. To address this challenge, we developed a simple physical powder-mixing strategy by mechanically mixing iron-based FTS catalysts with oxides such as SiO<sub>2</sub>, MgO, ZnO, ZrO<sub>2</sub>, MnO<sub>2</sub>, Al<sub>2</sub>O<sub>3</sub>, and graphene oxide (GO). Experimental results demonstrate that oxide incorporation significantly suppresses carbon deposition in a composition-dependent manner, thereby enhancing catalytic stability. Notably, after mixing with SiO<sub>2</sub> or MgO powder, the CO conversion reached 96.6% and 97.6%, respectively, maintaining stability for more than 20 h. In contrast, catalyst mixed with quartz sand particles underwent rapid deactivation within 20, with a decrease in CO conversion from 93.0% to 14.6%, accompanied by a sharp rise in CH<sub>4</sub> selectivity. By combining various characterization methods such as XRD, Mossbauer spectroscopy, TGA, XPS and CO-TPD, the promoting mechanism of oxides on reaction stability was deeply studied. The results indicate that the catalyst mixed SiO<sub>2</sub> powder reduced the content of active χ-Fe<sub>5</sub>C<sub>2</sub> phases from 97% to 52.1% and effectively suppressed carbon deposition. This enhancement is attributed to the strong interfacial interactions between SiO<sub>2</sub> and the iron-based catalyst, which moderately inhibited CO adsorption and dissociation kinetics, decelerated carbonization, and prevented rapid accumulation of carbon species on the catalyst surface. Similar mechanisms were observed over MgO additives, further validating the role of oxide-iron interactions. This work elucidates the mechanism of the interaction between iron-based catalysts and mixed oxides on carbon deposition behavior in Fischer-Tropsch synthesis reactions, providing an innovative strategy and theoretical foundation for designing highly active and stable catalysts.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 8","pages":"Pages 1212-1222"},"PeriodicalIF":0.0,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144886580","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}
Pub Date : 2025-08-01DOI: 10.1016/S1872-5813(25)60542-1
Hongyi CHEN, Anning ZHOU, Fuxin CHEN, Xinyu JIA, Yagang ZHANG, Mengdan MA, Jie LING, Wenlong LI
To address the issues of low yield and selectivity of benzaldehyde in the photocatalytic CO2-toluene reactions, a ZnTi-LDH photocatalyst with exposed hydroxyl groups was developed and a novel co-photocatalytic reaction system involving O2/CO2-toluene was established. The structure of ZnTi-LDH catalyst was characterized using XRD, FT-IR, N2 adsorption-desorption isotherms, XPS and other techniques. The effects of catalyst composition and O2/CO2 ratio on the yield and selectivity of benzaldehyde in the O2/CO2 co-photocatalytic oxidation of toluene were investigated in a pressurized reactor. The techniques and instruments such as isotope tracing, radical quenching, GC-MS, EPR, and others were employed to elucidate the free radical mechanism underlying the O2/CO2 synergistic photocatalytic oxidation of toluene. The results indicate that under solvent-free conditions, with a ZnTi-LDH catalyst composition of 3:1 (ZT-3:1) and an O2/CO2 ratio of 2:8, the irradiation by xenon light for 12 h yielded CO and benzaldehyde at rates of 121.37 and 947.89 μmol/(g·h), respectively, with selectivities of 96% and 60%. The total yield was 3.02 times higher than that of the CO2-toluene reaction alone. Selectivities for CO and benzaldehyde increased by 7% and 11%, respectively. These improvements are attributed primarily to the abundant −OH groups and high specific surface area of ZT-3:1, which promote the activation of CO2 adsorption on the catalyst, and the synergistic effect of O2 and CO2 expands the pathways for free radical reactions and improves the carrier utilization efficiency. This study provides a new approach to enhancing the CO2 conversion efficiency and co-producing the high-value-added products.
针对苯甲醛在光催化co2 -甲苯反应中产率低、选择性差的问题，研制了一种羟基暴露的ZnTi-LDH光催化剂，建立了一种新的O2/ co2 -甲苯共光催化反应体系。采用XRD、FT-IR、N2吸附-脱附等温线、XPS等技术对ZnTi-LDH催化剂的结构进行了表征。在加压反应器中研究了O2/CO2共光催化氧化甲苯反应中催化剂组成和O2/CO2比对苯甲醛收率和选择性的影响。采用同位素示踪、自由基猝灭、GC-MS、EPR等技术和仪器对O2/CO2协同光催化氧化甲苯的自由基机理进行了研究。结果表明，在无溶剂条件下，在ZnTi-LDH催化剂配比为3:1 （ZT-3:1）、O2/CO2比为2:8的条件下，氙灯照射12 h， CO和苯甲醛的产率分别为121.37和947.89 μmol/(g·h)，选择性分别为96%和60%。总产率是co2 -甲苯单独反应的3.02倍。对CO和苯甲醛的选择性分别提高了7%和11%。这些改善主要是由于丰富的−OH基团和ZT-3:1的高比表面积促进了CO2在催化剂上吸附的活化，O2和CO2的协同作用扩展了自由基反应的途径，提高了载体的利用效率。该研究为提高CO2转化效率和协同生产高附加值产品提供了一条新途径。
{"title":"Photocatalytic oxidation of toluene to benzaldehyde over exposed hydroxyl ZnTi-LDH nanosheets with O2/CO2","authors":"Hongyi CHEN, Anning ZHOU, Fuxin CHEN, Xinyu JIA, Yagang ZHANG, Mengdan MA, Jie LING, Wenlong LI","doi":"10.1016/S1872-5813(25)60542-1","DOIUrl":"10.1016/S1872-5813(25)60542-1","url":null,"abstract":"<div><div>To address the issues of low yield and selectivity of benzaldehyde in the photocatalytic CO<sub>2</sub>-toluene reactions, a ZnTi-LDH photocatalyst with exposed hydroxyl groups was developed and a novel co-photocatalytic reaction system involving O<sub>2</sub>/CO<sub>2</sub>-toluene was established. The structure of ZnTi-LDH catalyst was characterized using XRD, FT-IR, N<sub>2</sub> adsorption-desorption isotherms, XPS and other techniques. The effects of catalyst composition and O<sub>2</sub>/CO<sub>2</sub> ratio on the yield and selectivity of benzaldehyde in the O<sub>2</sub>/CO<sub>2</sub> co-photocatalytic oxidation of toluene were investigated in a pressurized reactor. The techniques and instruments such as isotope tracing, radical quenching, GC-MS, EPR, and others were employed to elucidate the free radical mechanism underlying the O<sub>2</sub>/CO<sub>2</sub> synergistic photocatalytic oxidation of toluene. The results indicate that under solvent-free conditions, with a ZnTi-LDH catalyst composition of 3:1 (ZT-3:1) and an O<sub>2</sub>/CO<sub>2</sub> ratio of 2:8, the irradiation by xenon light for 12 h yielded CO and benzaldehyde at rates of 121.37 and 947.89 μmol/(g·h), respectively, with selectivities of 96% and 60%. The total yield was 3.02 times higher than that of the CO<sub>2</sub>-toluene reaction alone. Selectivities for CO and benzaldehyde increased by 7% and 11%, respectively. These improvements are attributed primarily to the abundant −OH groups and high specific surface area of ZT-3:1, which promote the activation of CO<sub>2</sub> adsorption on the catalyst, and the synergistic effect of O<sub>2</sub> and CO<sub>2</sub> expands the pathways for free radical reactions and improves the carrier utilization efficiency. This study provides a new approach to enhancing the CO<sub>2</sub> conversion efficiency and co-producing the high-value-added products.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 8","pages":"Pages 1148-1161"},"PeriodicalIF":0.0,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144886495","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}
Pub Date : 2025-08-01DOI: 10.1016/S1872-5813(25)60541-X
Hongxing WANG , Lifeng CUI , Jie ZHANG , Shuhao WU , Shuai ZHANG , Ye TIAN , Xingang LI
γ-valerolactone (GVL) is a platform chemical derived from lignocellulose, which can be used as fuel additives, green solvent and feeding for the production of other high-value chemicals. Its efficient synthesis is of great significance for the development and utilization of biomass downstream products. Herein, with CuZnAl hydrotalcite as the precursor, a series of Cu-based catalysts with different Cu grain sizes were prepared by changing the aging temperature and used in the solvent-free gas-phase hydrogenation of ethyl levulinate (EL) to produce GVL. The Cu-based catalysts were systematically characterized by various techniques such as N2 sorption, XRD, SEM, TEM, H2-TPR, NH3-TPD, and in situ XPS, while the effect of Cu grain size on the performance of Cu-based catalyst in the EL hydrogenation was investigated. The results indicate that the electron cloud density of Cu as well as the Cu0/(Cu0+Cu+) ratio increase with a decrease of the Cu grain size; in addition, the Cu-based catalyst prepared by aging at a low temperature displays a large surface area and abundant acid sites. The synergistic effect of Cu0 sites and acid sites endows the Cu-based catalyst with superior performance in the EL hydrogenation to GVL. In particular, for the EL gas-phase hydrogenation under mild conditions (atmospheric pressure, 140 ℃, 0.3 h−1), the Cu-based catalyst prepared by aging at 30 ℃ achieves an EL conversion of 99.9% and a selectivity of 99.5% to GVL, with no significant deactivation observed in 240 h. The insight shown in this work should be meaningful for the large-scale production of GVL.
{"title":"Influence of Cu grain size on the performance of Cu-based catalyst in the gas-phase hydrogenation of ethyl levulinate","authors":"Hongxing WANG , Lifeng CUI , Jie ZHANG , Shuhao WU , Shuai ZHANG , Ye TIAN , Xingang LI","doi":"10.1016/S1872-5813(25)60541-X","DOIUrl":"10.1016/S1872-5813(25)60541-X","url":null,"abstract":"<div><div>γ-valerolactone (GVL) is a platform chemical derived from lignocellulose, which can be used as fuel additives, green solvent and feeding for the production of other high-value chemicals. Its efficient synthesis is of great significance for the development and utilization of biomass downstream products. Herein, with CuZnAl hydrotalcite as the precursor, a series of Cu-based catalysts with different Cu grain sizes were prepared by changing the aging temperature and used in the solvent-free gas-phase hydrogenation of ethyl levulinate (EL) to produce GVL. The Cu-based catalysts were systematically characterized by various techniques such as N<sub>2</sub> sorption, XRD, SEM, TEM, H<sub>2</sub>-TPR, NH<sub>3</sub>-TPD, and <em>in situ</em> XPS, while the effect of Cu grain size on the performance of Cu-based catalyst in the EL hydrogenation was investigated. The results indicate that the electron cloud density of Cu as well as the Cu<sup>0</sup>/(Cu<sup>0</sup>+Cu<sup>+</sup>) ratio increase with a decrease of the Cu grain size; in addition, the Cu-based catalyst prepared by aging at a low temperature displays a large surface area and abundant acid sites. The synergistic effect of Cu<sup>0</sup> sites and acid sites endows the Cu-based catalyst with superior performance in the EL hydrogenation to GVL. In particular, for the EL gas-phase hydrogenation under mild conditions (atmospheric pressure, 140 ℃, 0.3 h<sup>−1</sup>), the Cu-based catalyst prepared by aging at 30 ℃ achieves an EL conversion of 99.9% and a selectivity of 99.5% to GVL, with no significant deactivation observed in 240 h. The insight shown in this work should be meaningful for the large-scale production of GVL.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 8","pages":"Pages 1223-1232"},"PeriodicalIF":0.0,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144886498","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}
Pub Date : 2025-08-01DOI: 10.1016/S1872-5813(24)60531-1
Ruitao LI , Kun GONG , Yuanyuan DAI , Qiang NIU , Tiejun LIN , Liangshu ZHONG
CeO2 based semiconductor are widely used in solar-driven photothermal catalytic dry reforming of methane (DRM) reaction, but still suffer from low activity and low light utilization efficiency. This study developed graphite-CeO2 interfaces to enhance solar-driven photothermal catalytic DRM. Compared with carbon nanotubes-modified CeO2 (CeO2-CNT), graphite-modified CeO2 (CeO2-GRA) constructed graphite-CeO2 interfaces with distortion in CeO2, leading to the formation abundant oxygen vacancies. These graphite-CeO2 interfaces with oxygen vacancies enhanced optical absorption and promoted the generation and separation of photogenerated carriers. The high endothermic capacity of graphite elevated the catalyst surface temperature from 592.1−691.3 ℃, boosting light-to-thermal conversion. The synergy between photogenerated carriers and localized heat enabled Ni/CeO2-GRA to achieve a CO production rate of 9985.6 mmol/(g·h) (vs7192.4 mmol/(g·h) for Ni/ CeO2) and a light-to-fuel efficiency of 21.8% (vs13.8% for Ni/ CeO2). This work provides insights for designing graphite-semiconductor interfaces to advance photothermal catalytic efficiency.
{"title":"Constructing graphite-CeO2 interfaces to enhance the photothermal activity for solar-driven dry reforming of methane","authors":"Ruitao LI , Kun GONG , Yuanyuan DAI , Qiang NIU , Tiejun LIN , Liangshu ZHONG","doi":"10.1016/S1872-5813(24)60531-1","DOIUrl":"10.1016/S1872-5813(24)60531-1","url":null,"abstract":"<div><div>CeO<sub>2</sub> based semiconductor are widely used in solar-driven photothermal catalytic dry reforming of methane (DRM) reaction, but still suffer from low activity and low light utilization efficiency. This study developed graphite-CeO<sub>2</sub> interfaces to enhance solar-driven photothermal catalytic DRM. Compared with carbon nanotubes-modified CeO<sub>2</sub> (CeO<sub>2</sub>-CNT), graphite-modified CeO<sub>2</sub> (CeO<sub>2</sub>-GRA) constructed graphite-CeO<sub>2</sub> interfaces with distortion in CeO<sub>2</sub>, leading to the formation abundant oxygen vacancies. These graphite-CeO<sub>2</sub> interfaces with oxygen vacancies enhanced optical absorption and promoted the generation and separation of photogenerated carriers. The high endothermic capacity of graphite elevated the catalyst surface temperature from 592.1−691.3 ℃, boosting light-to-thermal conversion. The synergy between photogenerated carriers and localized heat enabled Ni/CeO<sub>2</sub>-GRA to achieve a CO production rate of 9985.6 mmol/(g·h) (<em>vs</em>7192.4 mmol/(g·h) for Ni/ CeO<sub>2</sub>) and a light-to-fuel efficiency of 21.8% (<em>vs</em>13.8% for Ni/ CeO<sub>2</sub>). This work provides insights for designing graphite-semiconductor interfaces to advance photothermal catalytic efficiency.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 8","pages":"Pages 1137-1147"},"PeriodicalIF":0.0,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144886581","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}
Pub Date : 2025-08-01DOI: 10.1016/S1872-5813(25)60576-7
Fengren ZHANG , Ying YAN , Feng LIU , Yang WU , Shuqin LIANG , Huifang CHENG , Shanlei HAN , LIU Jixing , Wenshuai ZHU
Catalytic oxidation desulfurization (CODS) technology has shown great promise for diesel desulfurization by virtue of its low cost, mild reaction conditions, and superior desulfurization performance. Herein, a series of FeMoOx/LaTiOy-z samples with diverse Fe/Mo ratios were prepared via a facile citric acid-assisted method. The impact of Fe incorporation on the dispersion and surface elemental states of Mo species, as well as oxygen species content of the synthesized FeMoOx/LaTiOy-z catalysts were systematically characterized using TEM, BET, UV-vis DRS, XPS, XANES, and reaction kinetics, and their CODS performances were examined for 4,6-DMDBT removal. Experimental results demonstrated that Fe/Mo ratio significantly affected the Ti−O bond strength, surface dispersion and electronic structure of Mo species on FeMoOx/LaTiOy-z catalysts. FeMoOx/LaTiOy-2 catalyst showed outstanding cycling durability and the best CODS performance with almost 100% removal of 4,6-DMDBT from model oil within 75 min due to its proper MoO3 dispersion, optimal redox property, and the most oxygen vacancy concentration. Nevertheless, further enhancing Fe content led to the increased dispersion of Mo species, while the decrease active Mo species as well as the increase of steric effect for 4,6-DMDBT accessing to the catalytic reactive sites considerably increase the apparent activation energy of FeMoOx/LaTiOy-z (z> 2) catalysts during the CODS process, thereby seriously suppressing their CODS performances. Moreover, Radical trapping experiments reveal that the ·, generated by the activation of O2 at the active sites, catalytic oxidized 4,6-DMDBT to the product of 4,6-DMDBTO2, thereby enabling both deep desulfurization and recovery of high-value 4,6-DMDBTO2. These findings offer an alternative strategy to achieve ultra deep desulfurization as well as separate and recover high economic value sulfone substances from diesel.
{"title":"Regulating the Fe/Mo ratio of FeMoOx/LaTiOy to boost aerobic oxidative desulfurization of diesel","authors":"Fengren ZHANG , Ying YAN , Feng LIU , Yang WU , Shuqin LIANG , Huifang CHENG , Shanlei HAN , LIU Jixing , Wenshuai ZHU","doi":"10.1016/S1872-5813(25)60576-7","DOIUrl":"10.1016/S1872-5813(25)60576-7","url":null,"abstract":"<div><div>Catalytic oxidation desulfurization (CODS) technology has shown great promise for diesel desulfurization by virtue of its low cost, mild reaction conditions, and superior desulfurization performance. Herein, a series of FeMoO<sub><em>x</em></sub>/LaTiO<sub><em>y</em></sub>-<em>z</em> samples with diverse Fe/Mo ratios were prepared via a facile citric acid-assisted method. The impact of Fe incorporation on the dispersion and surface elemental states of Mo species, as well as oxygen species content of the synthesized FeMoO<sub><em>x</em></sub>/LaTiO<sub><em>y</em></sub>-<em>z</em> catalysts were systematically characterized using TEM, BET, UV-vis DRS, XPS, XANES, and reaction kinetics, and their CODS performances were examined for 4,6-DMDBT removal. Experimental results demonstrated that Fe/Mo ratio significantly affected the Ti−O bond strength, surface dispersion and electronic structure of Mo species on FeMoO<sub><em>x</em></sub>/LaTiO<sub><em>y</em></sub>-<em>z</em> catalysts. FeMoO<sub><em>x</em></sub>/LaTiO<sub><em>y</em></sub>-2 catalyst showed outstanding cycling durability and the best CODS performance with almost 100% removal of 4,6-DMDBT from model oil within 75 min due to its proper MoO<sub>3</sub> dispersion, optimal redox property, and the most oxygen vacancy concentration. Nevertheless, further enhancing Fe content led to the increased dispersion of Mo species, while the decrease active Mo species as well as the increase of steric effect for 4,6-DMDBT accessing to the catalytic reactive sites considerably increase the apparent activation energy of FeMoO<sub><em>x</em></sub>/LaTiO<sub><em>y</em></sub>-<em>z</em> (<em>z</em>> 2) catalysts during the CODS process, thereby seriously suppressing their CODS performances. Moreover, Radical trapping experiments reveal that the ·, generated by the activation of O<sub>2</sub> at the active sites, catalytic oxidized 4,6-DMDBT to the product of 4,6-DMDBTO<sub>2</sub>, thereby enabling both deep desulfurization and recovery of high-value 4,6-DMDBTO<sub>2</sub>. These findings offer an alternative strategy to achieve ultra deep desulfurization as well as separate and recover high economic value sulfone substances from diesel.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 8","pages":"Pages 1255-1268"},"PeriodicalIF":0.0,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144886497","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}
Pub Date : 2025-08-01DOI: 10.1016/S1872-5813(25)60537-8
Xiaoqian BAN, Kai WANG, Yonghong LU, Haibo XU
Carbon fiber has been commercially applied as a cathode material in dissolved oxygen-seawater batteries (DO-SWB). However, the low concentration of dissolved oxygen in seawater and the limited activity of the oxygen reduction reaction (ORR) restrict the improvement of battery power density. In recent years, nitrogen doping of carbon materials has attracted significant research interest. In this work, aniline(An) was used as the nitrogen source, and nitrogen-doped electrodes were prepared via a one-step electrochemical treatment of polyacrylonitrile-based carbon fiber (PAN-CF) in a mixed solution of An and H2SO4 under optimized process conditions. The electrodes were characterized using scanning electron microscopy (SEM), Raman spectrum (Raman), and X-ray photoelectron spectroscopy (XPS), combined with electrochemical testing methods to evaluate the surface characteristics and ORR activity of the electrodes, followed by an analysis of the underlying mechanism. Electrochemical modification introduced defects on the carbon fiber surface and generated pyridinic functional groups, effectively regulating the electronic structure of the carbon material, increasing the number of active sites on the electrode surface, and enhancing oxygen adsorption and charge transfer capabilities. As a result, the nitrogen-doped electrode exhibited excellent ORR performance. The optimal electrode achieved an ORR onset potential of −0.12 VvsSCE and an ORRspecific current density of 510 mA/gat −0.4 VvsSCE, indicating promising application prospects as a cathode material for DO-SWB.
{"title":"Nitrogen-doped modification of carbon fiber cathode with aniline for oxygen reduction catalysis in dissolved oxygen seawater battery","authors":"Xiaoqian BAN, Kai WANG, Yonghong LU, Haibo XU","doi":"10.1016/S1872-5813(25)60537-8","DOIUrl":"10.1016/S1872-5813(25)60537-8","url":null,"abstract":"<div><div>Carbon fiber has been commercially applied as a cathode material in dissolved oxygen-seawater batteries (DO-SWB). However, the low concentration of dissolved oxygen in seawater and the limited activity of the oxygen reduction reaction (ORR) restrict the improvement of battery power density. In recent years, nitrogen doping of carbon materials has attracted significant research interest. In this work, aniline(An) was used as the nitrogen source, and nitrogen-doped electrodes were prepared via a one-step electrochemical treatment of polyacrylonitrile-based carbon fiber (PAN-CF) in a mixed solution of An and H<sub>2</sub>SO<sub>4</sub> under optimized process conditions. The electrodes were characterized using scanning electron microscopy (SEM), Raman spectrum (Raman), and X-ray photoelectron spectroscopy (XPS), combined with electrochemical testing methods to evaluate the surface characteristics and ORR activity of the electrodes, followed by an analysis of the underlying mechanism. Electrochemical modification introduced defects on the carbon fiber surface and generated pyridinic functional groups, effectively regulating the electronic structure of the carbon material, increasing the number of active sites on the electrode surface, and enhancing oxygen adsorption and charge transfer capabilities. As a result, the nitrogen-doped electrode exhibited excellent ORR performance. The optimal electrode achieved an ORR onset potential of −0.12 V<em>vs</em>SCE and an ORRspecific current density of 510 mA/gat −0.4 V<em>vs</em>SCE, indicating promising application prospects as a cathode material for DO-SWB.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 8","pages":"Pages 1183-1190"},"PeriodicalIF":0.0,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144886578","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}
Pub Date : 2025-08-01DOI: 10.1016/S1872-5813(25)60533-0
Ting HUANG , Bing FENG , Peipei LU , Zhongliang ZHANG , Qi NIU , Zonghu MA , Kai LI , Qiang LU
To optimize the CO2 adsorption performance of carbon materials, this study proposed a preparation method for biomass-based porous carbon through hydrothermal carbonization coupled with nitrogen source optimization and K2CO3 activation. The effects of different nitrogen sources (urea, piperazine, melamine, and polyaniline) and activation temperatures on the physicochemical features and CO2 adsorption characteristics of the porous carbons were systematically investigated. The results indicated that different nitrogen sources showed varying impacts on the CO2 uptake of porous carbons, and not all nitrogen sources enhanced the adsorption performance. The urea and piperazine doped porous carbons exhibited relatively low nitrogen contents and specific surface areas. Whereas the melamine doped carbons showed higher nitrogen contents and specific surface areas, but lacked narrow micropores, limiting their CO2 adsorption performance. In contrast, PAC-700, prepared using polyaniline as nitrogen source, featured a well-developed pore structure, abundant narrow micropores and pyrrolic-N groups, endowing it with enhanced CO2 adsorption capability. At 0 °C/1 bar and 25 °C/1 bar, the CO2 uptake of PAC-700 reached 6.85 and 4.64 mmol/g, respectively. Additionally, PAC-700 maintained a CO2 uptake retention ratio of 99% after 5 adsorption-desorption cycles and exhibited good CO2/N2 selectivity of 22.4−51.6. These findings highlighted the advantageous CO2 adsorption performance of PAC-700, indicating its substantial application potential in the domain of carbon capture.
{"title":"Hydrothermal N-doping assisted synthesis of poplar sawdust-derived porous carbons for carbon capture","authors":"Ting HUANG , Bing FENG , Peipei LU , Zhongliang ZHANG , Qi NIU , Zonghu MA , Kai LI , Qiang LU","doi":"10.1016/S1872-5813(25)60533-0","DOIUrl":"10.1016/S1872-5813(25)60533-0","url":null,"abstract":"<div><div>To optimize the CO<sub>2</sub> adsorption performance of carbon materials, this study proposed a preparation method for biomass-based porous carbon through hydrothermal carbonization coupled with nitrogen source optimization and K<sub>2</sub>CO<sub>3</sub> activation. The effects of different nitrogen sources (urea, piperazine, melamine, and polyaniline) and activation temperatures on the physicochemical features and CO<sub>2</sub> adsorption characteristics of the porous carbons were systematically investigated. The results indicated that different nitrogen sources showed varying impacts on the CO<sub>2</sub> uptake of porous carbons, and not all nitrogen sources enhanced the adsorption performance. The urea and piperazine doped porous carbons exhibited relatively low nitrogen contents and specific surface areas. Whereas the melamine doped carbons showed higher nitrogen contents and specific surface areas, but lacked narrow micropores, limiting their CO<sub>2</sub> adsorption performance. In contrast, PAC-700, prepared using polyaniline as nitrogen source, featured a well-developed pore structure, abundant narrow micropores and pyrrolic-N groups, endowing it with enhanced CO<sub>2</sub> adsorption capability. At 0 °C/1 bar and 25 °C/1 bar, the CO<sub>2</sub> uptake of PAC-700 reached 6.85 and 4.64 mmol/g, respectively. Additionally, PAC-700 maintained a CO<sub>2</sub> uptake retention ratio of 99% after 5 adsorption-desorption cycles and exhibited good CO<sub>2</sub>/N<sub>2</sub> selectivity of 22.4−51.6. These findings highlighted the advantageous CO<sub>2</sub> adsorption performance of PAC-700, indicating its substantial application potential in the domain of carbon capture.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 8","pages":"Pages 1191-1202"},"PeriodicalIF":0.0,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144886579","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}
Pub Date : 2025-08-01DOI: 10.1016/S1872-5813(25)60544-5
Lei ZHANG , Mingxin LIU , Yisong ZHENG , Guochao AN , Jiao HAN , Caishun ZHANG , Zhixian GAO
Using CeO2, ZrO2, γ-Al2O3, AlO(OH) as the carrier and RuCl3 as the ruthenium source, the Ru/MxOy catalyst was prepared by deposition-precipitation method. Through XRD, BET, H2-TPR, XPS and other characterization methods, combined with high flux methanol steam reforming hydrogen production reaction evaluation, the influence of different carriers on the catalytic performance of Ru/MxOy catalyst was investigated. The experimental results showed that the difference of the interaction between RuOx and the carrier, as well as the presence or absence of oxygen vacancy, showed a significant carrier effect. The Ru/CeO2 catalyst prepared with CeO2 as the carrier has good dispersibility of RuOx, strong interaction between RuOx and the carrier, oxygen vacancy, and good catalytic activity. At the reaction temperature of 420 ℃, the molar ratio of water to alcohol is 1.2, and the space velocity of methanol water mass is 6 h−1, the methanol conversion rate is 88.64%, and the catalytic activity is good at high flux.
{"title":"Carrier effect of Ru/MxOy catalyzed methanol steam reforming reaction","authors":"Lei ZHANG , Mingxin LIU , Yisong ZHENG , Guochao AN , Jiao HAN , Caishun ZHANG , Zhixian GAO","doi":"10.1016/S1872-5813(25)60544-5","DOIUrl":"10.1016/S1872-5813(25)60544-5","url":null,"abstract":"<div><div>Using CeO<sub>2</sub>, ZrO<sub>2</sub>, <em>γ</em>-Al<sub>2</sub>O<sub>3</sub>, AlO(OH) as the carrier and RuCl<sub>3</sub> as the ruthenium source, the Ru/M<sub><em>x</em></sub>O<sub><em>y</em></sub> catalyst was prepared by deposition-precipitation method. Through XRD, BET, H<sub>2</sub>-TPR, XPS and other characterization methods, combined with high flux methanol steam reforming hydrogen production reaction evaluation, the influence of different carriers on the catalytic performance of Ru/M<sub><em>x</em></sub>O<sub><em>y</em></sub> catalyst was investigated. The experimental results showed that the difference of the interaction between RuO<sub><em>x</em></sub> and the carrier, as well as the presence or absence of oxygen vacancy, showed a significant carrier effect. The Ru/CeO<sub>2</sub> catalyst prepared with CeO<sub>2</sub> as the carrier has good dispersibility of RuO<sub><em>x</em></sub>, strong interaction between RuO<sub><em>x</em></sub> and the carrier, oxygen vacancy, and good catalytic activity. At the reaction temperature of 420 ℃, the molar ratio of water to alcohol is 1.2, and the space velocity of methanol water mass is 6 h<sup>−1</sup>, the methanol conversion rate is 88.64%, and the catalytic activity is good at high flux.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 8","pages":"Pages 1233-1242"},"PeriodicalIF":0.0,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144886499","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}
Pub Date : 2025-07-01DOI: 10.1016/S1872-5813(24)60523-2
Kunyun WU , Shiyu SU , Xia WANG , Yingqi ZHAO , Caishun ZHANG , Jiao HAN , Yuehong ZHANG , Xiaoning HOU , Lei ZHANG , Zhixian GAO
In this paper, three methods, namely hydrothermal, Al modification and acid washing, were used to modify Cu-Al spinel catalyst, and then the catalysts were characterized by XRD, BET, H2-TPR and XPS techniques. In conjunction with the performances of methanol steam reforming, the effects of surface composition and structure on the catalytic behaviors of the sustained release process were investigated. The results showed that new crystalline phase formed and surface species changed after the hydrothermal treatment, while Al-modification and acid-treated catalysts didn't change the crystalline phase composition, but the surface Al/Cu ratio and the distribution of Cu species changed. Based on the characterization data of the released Cu, it could be inferred that all the three treatments led to variations of the microscopic surface structure, thus exhibiting different sustained release catalytic behaviors. Specifically, the hydrothermal treatment enhanced the catalytic activity, while Al-modification and acid-treated catalysts showed inferior activity but showing obvious sustained release behavior. The findings of this paper provide a basis for further studies on the surface modification of the Cu-Al spinel catalyst.
{"title":"Characteristics of the sustained release of Cu-Al spinel pretreated by different methods for hydrogen production from methanol steam reforming","authors":"Kunyun WU , Shiyu SU , Xia WANG , Yingqi ZHAO , Caishun ZHANG , Jiao HAN , Yuehong ZHANG , Xiaoning HOU , Lei ZHANG , Zhixian GAO","doi":"10.1016/S1872-5813(24)60523-2","DOIUrl":"10.1016/S1872-5813(24)60523-2","url":null,"abstract":"<div><div>In this paper, three methods, namely hydrothermal, Al modification and acid washing, were used to modify Cu-Al spinel catalyst, and then the catalysts were characterized by XRD, BET, H<sub>2</sub>-TPR and XPS techniques. In conjunction with the performances of methanol steam reforming, the effects of surface composition and structure on the catalytic behaviors of the sustained release process were investigated. The results showed that new crystalline phase formed and surface species changed after the hydrothermal treatment, while Al-modification and acid-treated catalysts didn't change the crystalline phase composition, but the surface Al/Cu ratio and the distribution of Cu species changed. Based on the characterization data of the released Cu, it could be inferred that all the three treatments led to variations of the microscopic surface structure, thus exhibiting different sustained release catalytic behaviors. Specifically, the hydrothermal treatment enhanced the catalytic activity, while Al-modification and acid-treated catalysts showed inferior activity but showing obvious sustained release behavior. The findings of this paper provide a basis for further studies on the surface modification of the Cu-Al spinel catalyst.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"53 7","pages":"Pages 1050-1060"},"PeriodicalIF":0.0,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144696624","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}
扫码关注我们
求助内容：
应助结果提醒方式：
京公网安备 11010802042870号