Pub Date : 2026-02-01DOI: 10.1016/S1872-5813(25)60601-3
Lu LIU, Shenyong REN, Chengshu YAO, Baojian SHEN, Chunming XU
Catalytic decomposition of methane, which produces high-purity hydrogen and high-value-added carbon nanomaterials, has shown considerable potential for development and is expected to yield significant economic benefits in the future. However, designing catalysts that simultaneously exhibit high activity and long-term stability remains a significant challenge. Tuning the catalyst's structure and electronic properties is an effective strategy for enhancing the reaction performance. In this work, a series of NixZr/ZSM-5 catalysts were prepared using the incipient wetness impregnation method, and the effect of Zr loadings on catalyst properties and performance was systematically investigated. The calcined and reduced catalysts were characterized by low-temperature N2 adsorption-desorption, XRD, SEM, H2-TPR and XPS. The results showed that the addition of Zr significantly increased the specific surface area of the catalyst and reduced the metal particle size. Smaller NiO particles were found to enter the pores of the HZSM-5 support, and electronic interactions between NiO and ZrO2 markedly enhanced the metal-support interaction. The catalyst exhibited optimal catalytic performance at a Zr loading of 5%, achieving a maximum methane conversion of 68% at 625 °C, maintaining activity for 900 min, and delivering a carbon yield of 1927%. Further increasing the Zr loading yielded only limited improvements in catalytic performance. Characterization of the spent catalysts and carbon products via TEM, Raman spectroscopy, and TGA revealed that the introduction of ZrO2 reduced metal sintering and promoted a shift in carbon nanofibers growth mode from tip-growth to base-growth. The mechanism of base-growth enabled the catalyst to maintain reaction activity for an extended period.
{"title":"The role of Zr in modulating the electronic and structural properties of supported Ni catalysts for catalytic decomposition of methane","authors":"Lu LIU, Shenyong REN, Chengshu YAO, Baojian SHEN, Chunming XU","doi":"10.1016/S1872-5813(25)60601-3","DOIUrl":"10.1016/S1872-5813(25)60601-3","url":null,"abstract":"<div><div>Catalytic decomposition of methane, which produces high-purity hydrogen and high-value-added carbon nanomaterials, has shown considerable potential for development and is expected to yield significant economic benefits in the future. However, designing catalysts that simultaneously exhibit high activity and long-term stability remains a significant challenge. Tuning the catalyst's structure and electronic properties is an effective strategy for enhancing the reaction performance. In this work, a series of Ni<em>x</em>Zr/ZSM-5 catalysts were prepared using the incipient wetness impregnation method, and the effect of Zr loadings on catalyst properties and performance was systematically investigated. The calcined and reduced catalysts were characterized by low-temperature N<sub>2</sub> adsorption-desorption, XRD, SEM, H<sub>2</sub>-TPR and XPS. The results showed that the addition of Zr significantly increased the specific surface area of the catalyst and reduced the metal particle size. Smaller NiO particles were found to enter the pores of the HZSM-5 support, and electronic interactions between NiO and ZrO<sub>2</sub> markedly enhanced the metal-support interaction. The catalyst exhibited optimal catalytic performance at a Zr loading of 5%, achieving a maximum methane conversion of 68% at 625 °C, maintaining activity for 900 min, and delivering a carbon yield of 1927%. Further increasing the Zr loading yielded only limited improvements in catalytic performance. Characterization of the spent catalysts and carbon products via TEM, Raman spectroscopy, and TGA revealed that the introduction of ZrO<sub>2</sub> reduced metal sintering and promoted a shift in carbon nanofibers growth mode from tip-growth to base-growth. The mechanism of base-growth enabled the catalyst to maintain reaction activity for an extended period.\u0000\t\t\t\t<span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (142KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 2","pages":"Article 20250192"},"PeriodicalIF":0.0,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172912","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 : 2026-02-01DOI: 10.1016/S1872-5813(25)60602-5
Peng WANG , Changqing DONG , Junjie XUE , Qi GAO , Xiaoying HU , Junjiao ZHANG , Jie ZHAO
Oxygen carriers play a fundamental role in chemical looping combustion (CLC). Iron-based carriers have been extensively investigated owing to their abundance and environmentally friendly. However, the reactivity and separability of iron-based carriers require further enhancement. This study investigates the effect of the concentration of Mn doping on reactivity, elastic properties and magnetic properties based on density functional theory (DFT) calculations. Theoretical results demonstrate that Mn doping effectively enhances reactivity by reducing the oxygen vacancy formation energy (Evac) from 2.33 to 0.87 eV. However, Mn doping introduces lattice distortions that deteriorate elastic properties, thereby reducing wear resistance, as evidenced by a 54.54% decrease in the hardness-to-Young's modulus ratio (HV/EV) for α-Fe2O3 and an 83.33% reduction for Fe3O4. Furthermore, Mn doping also modifies magnetic properties. The maximum of saturation magnetization (Ms) of Fe3O4 reaches 121.02 emu/g at 33.33% Mn doping concentration. Finally, systematic evaluation identifies 33.33% as the optimal Mn doping concentration, achieving a balance in enhanced reactivity, superior magnetic performance, and retained elastic stability.
{"title":"Effects of Mn doping on the reactivity, elastic, and magnetic properties of α-Fe2O3 based on DFT calculation","authors":"Peng WANG , Changqing DONG , Junjie XUE , Qi GAO , Xiaoying HU , Junjiao ZHANG , Jie ZHAO","doi":"10.1016/S1872-5813(25)60602-5","DOIUrl":"10.1016/S1872-5813(25)60602-5","url":null,"abstract":"<div><div>Oxygen carriers play a fundamental role in chemical looping combustion (CLC). Iron-based carriers have been extensively investigated owing to their abundance and environmentally friendly. However, the reactivity and separability of iron-based carriers require further enhancement. This study investigates the effect of the concentration of Mn doping on reactivity, elastic properties and magnetic properties based on density functional theory (DFT) calculations. Theoretical results demonstrate that Mn doping effectively enhances reactivity by reducing the oxygen vacancy formation energy (E<sub>vac</sub>) from 2.33 to 0.87 eV. However, Mn doping introduces lattice distortions that deteriorate elastic properties, thereby reducing wear resistance, as evidenced by a 54.54% decrease in the hardness-to-Young's modulus ratio (<em>H</em><sub>V</sub>/<em>E</em><sub>V</sub>) for α-Fe<sub>2</sub>O<sub>3</sub> and an 83.33% reduction for Fe<sub>3</sub>O<sub>4</sub>. Furthermore, Mn doping also modifies magnetic properties. The maximum of saturation magnetization (<em>M</em><sub>s</sub>) of Fe<sub>3</sub>O<sub>4</sub> reaches 121.02 emu/g at 33.33% Mn doping concentration. Finally, systematic evaluation identifies 33.33% as the optimal Mn doping concentration, achieving a balance in enhanced reactivity, superior magnetic performance, and retained elastic stability.\u0000\t\t\t\t<span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (92KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 2","pages":"Article 20250180"},"PeriodicalIF":0.0,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146172829","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 : 2026-01-01DOI: 10.1016/S1872-5813(25)60590-1
Jingzhou WANG, Chenzhong YAO, Xisheng ZHANG, Ziwei MA, Linfeng LI
In this study, a straightforward one-step hydrothermal method was successfully utilized to synthesize the solid solution Na0.9Mg0.45Ti3.55O8-Na2Ni2Ti6O16 (NNMTO-x), where x denotes the molar percentage of Na2Ni2Ti6O16 (NNTO) within Na0.9Mg0.45Ti3.55O8 (NMTO), with x values of 10, 20, 30, 40, and 50. Both XPS (X-ray Photoelectron Spectroscopy) and EDX (Energy Dispersive X-ray Spectroscopy) analyses unequivocally validated the formation of the NNMTO-x solid solutions. It was observed that when x is below 40, the NNMTO-x solid solution retains the structural characteristics of the original NMTO. However, beyond this threshold, significant alterations in crystal morphology were noted, accompanied by a noticeable decline in photocatalytic activity. Notably, the absorption edge of NNMTO-x (x<40) exhibited a shift towards the visible-light spectrum, thereby substantially broadening the absorption range. The findings highlight that NNMTO-30 possesses the most pronounced photocatalytic activity for the reduction of CO2. Specifically, after a 6 h irradiation period, the production rates of CO and CH4 were recorded at 42.38 and 1.47 μmol/g, respectively. This investigation provides pivotal insights that are instrumental in the advancement of highly efficient and stable photocatalysts tailored for CO2 reduction processes.
{"title":"Facile synthesis of Na0.9Mg0.45Ti3.55O8-Na2Ni2Ti6O16 solid solutions for improving photocatalytic CO2 reduction","authors":"Jingzhou WANG, Chenzhong YAO, Xisheng ZHANG, Ziwei MA, Linfeng LI","doi":"10.1016/S1872-5813(25)60590-1","DOIUrl":"10.1016/S1872-5813(25)60590-1","url":null,"abstract":"<div><div>In this study, a straightforward one-step hydrothermal method was successfully utilized to synthesize the solid solution Na<sub>0.9</sub>Mg<sub>0.45</sub>Ti<sub>3.55</sub>O<sub>8</sub>-Na<sub>2</sub>Ni<sub>2</sub>Ti<sub>6</sub>O<sub>16</sub> (NNMTO-<em>x</em>), where <em>x</em> denotes the molar percentage of Na<sub>2</sub>Ni<sub>2</sub>Ti<sub>6</sub>O<sub>16</sub> (NNTO) within Na<sub>0.9</sub>Mg<sub>0.45</sub>Ti<sub>3.55</sub>O<sub>8</sub> (NMTO), with <em>x</em> values of 10, 20, 30, 40, and 50. Both XPS (X-ray Photoelectron Spectroscopy) and EDX (Energy Dispersive X-ray Spectroscopy) analyses unequivocally validated the formation of the NNMTO-<em>x</em> solid solutions. It was observed that when <em>x</em> is below 40, the NNMTO-<em>x</em> solid solution retains the structural characteristics of the original NMTO. However, beyond this threshold, significant alterations in crystal morphology were noted, accompanied by a noticeable decline in photocatalytic activity. Notably, the absorption edge of NNMTO-<em>x</em> (<em>x</em><40) exhibited a shift towards the visible-light spectrum, thereby substantially broadening the absorption range. The findings highlight that NNMTO-30 possesses the most pronounced photocatalytic activity for the reduction of CO<sub>2</sub>. Specifically, after a 6 h irradiation period, the production rates of CO and CH<sub>4</sub> were recorded at 42.38 and 1.47 μmol/g, respectively. This investigation provides pivotal insights that are instrumental in the advancement of highly efficient and stable photocatalysts tailored for CO<sub>2</sub> reduction processes.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 1","pages":"Pages 1-11"},"PeriodicalIF":0.0,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957656","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 : 2026-01-01DOI: 10.1016/S1872-5813(25)60594-9
Qi WANG , Lifang CHEN , Ruimin DING , Xi YIN
Hydrogen peroxide (H2O2) oxidation and reduction reactions (HPOR/HPRR) are pivotal in various innovative electrochemical energy conversion devices. A comprehensive understanding of these mechanisms is critical for catalyst design and performance improvement in these applications. In this work, we systematically investigate the HPOR/HPRR mechanisms on low-index Pt surfaces, specifically Pt(111), Pt(100) and Pt(110), through density functional theory (DFT) calculations combined with the computational hydrogen electrode (CHE) model. For HPOR, all the low-index Pt surfaces exhibit a unified potential-determining step (PDS) involving the electrochemical oxidation of hydroperoxyl intermediates (HOO*). The binding free energy of HOO* (ΔGHOO*) emerges as an activity descriptor, with Pt(110) exhibiting the highest HPOR activity. The HPRR mechanism follows a chem-electrochemical (C-EC) pathway. The rate-determining step (RDS) of HPRR is either the cleavage of the HO–OH bond (chemical) or the reduction of HO (electrochemical), depending on their respective activation energies. These activation energies are functions of the HO* binding free energy, ΔGHO*, establishing ΔGHO* as the descriptor for HPRR activity prediction. Pt(111) and Pt(100) are identified as the most active HPRR catalysts among the studied metal surfaces, although they still experience a significant overpotential. The scaling relationship between ΔGHOO* and ΔGHO* reveals a thermodynamic coupling of HPOR and HPRR, explaining their occurrence on Pt surfaces. These findings provide important insights and activity descriptors for both HPOR and HPRR, providing valuable guidance for the design of electrocatalysts in H2O2-related energy applications and fuel cells.
{"title":"Theoretical insights into the hydrogen peroxide oxidation and reduction reactions on low-index Pt surfaces","authors":"Qi WANG , Lifang CHEN , Ruimin DING , Xi YIN","doi":"10.1016/S1872-5813(25)60594-9","DOIUrl":"10.1016/S1872-5813(25)60594-9","url":null,"abstract":"<div><div>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) oxidation and reduction reactions (HPOR/HPRR) are pivotal in various innovative electrochemical energy conversion devices. A comprehensive understanding of these mechanisms is critical for catalyst design and performance improvement in these applications. In this work, we systematically investigate the HPOR/HPRR mechanisms on low-index Pt surfaces, specifically Pt(111), Pt(100) and Pt(110), through density functional theory (DFT) calculations combined with the computational hydrogen electrode (CHE) model. For HPOR, all the low-index Pt surfaces exhibit a unified potential-determining step (PDS) involving the electrochemical oxidation of hydroperoxyl intermediates (HOO*). The binding free energy of HOO* (Δ<em>G</em><sub>HOO*</sub>) emerges as an activity descriptor, with Pt(110) exhibiting the highest HPOR activity. The HPRR mechanism follows a chem-electrochemical (C-EC) pathway. The rate-determining step (RDS) of HPRR is either the cleavage of the HO–OH bond (chemical) or the reduction of HO (electrochemical), depending on their respective activation energies. These activation energies are functions of the HO* binding free energy, Δ<em>G</em><sub>HO*</sub>, establishing Δ<em>G</em><sub>HO*</sub> as the descriptor for HPRR activity prediction. Pt(111) and Pt(100) are identified as the most active HPRR catalysts among the studied metal surfaces, although they still experience a significant overpotential. The scaling relationship between Δ<em>G</em><sub>HOO*</sub> and Δ<em>G</em><sub>HO*</sub> reveals a thermodynamic coupling of HPOR and HPRR, explaining their occurrence on Pt surfaces. These findings provide important insights and activity descriptors for both HPOR and HPRR, providing valuable guidance for the design of electrocatalysts in H<sub>2</sub>O<sub>2</sub>-related energy applications and fuel cells.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 1","pages":"Pages 1-11"},"PeriodicalIF":0.0,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957657","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 : 2026-01-01DOI: 10.1016/S1872-5813(25)60597-4
Haiting ZHAO, Zheng YAN, Yang LIU, Longde JIANG, Jingde LUAN
The efficiency and stability of catalysts for photocatalytic hydrogen evolution (PHE) are largely governed by the charge transfer behaviors across the heterojunction interfaces. In this study, CuO, a typical semiconductor featuring a broad spectral absorption range, is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction. The optimized photocatalyst (CdS-CuO2:1) delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h), 4.15-fold higher compared with bare CdS. X-ray photoelectron spectroscopy (XPS) and ultraviolet-visible diffuse reflection absorption spectroscopy (UV-vis DRS) confirmed the S-scheme band structure of the composites. Moreover, the surface photovoltage (SPV) and electron paramagnetic resonance (EPR) indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2:1 were respectively transferred to the conduction band (CB) of CdS with a higher reduction potential and the valence band (VB) of CuO with a higher oxidation potential under illumination, as expected for the S-scheme mechanism. Density-functional-theory calculations of the electron density difference (EDD) disclose an interfacial electric field oriented from CdS to CuO. This built-in field suppresses charge recombination and accelerates carrier migration, rationalizing the markedly enhanced PHE activity. This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-to-hydrogen conversion.
{"title":"S-scheme unidirectional transmission of CdS-CuO heterojunction benefits for superior photocatalytic hydrogen evolution efficiency","authors":"Haiting ZHAO, Zheng YAN, Yang LIU, Longde JIANG, Jingde LUAN","doi":"10.1016/S1872-5813(25)60597-4","DOIUrl":"10.1016/S1872-5813(25)60597-4","url":null,"abstract":"<div><div>The efficiency and stability of catalysts for photocatalytic hydrogen evolution (PHE) are largely governed by the charge transfer behaviors across the heterojunction interfaces. In this study, CuO, a typical semiconductor featuring a broad spectral absorption range, is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction. The optimized photocatalyst (CdS-CuO2:1) delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h), 4.15-fold higher compared with bare CdS. X-ray photoelectron spectroscopy (XPS) and ultraviolet-visible diffuse reflection absorption spectroscopy (UV-vis DRS) confirmed the S-scheme band structure of the composites. Moreover, the surface photovoltage (SPV) and electron paramagnetic resonance (EPR) indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2:1 were respectively transferred to the conduction band (CB) of CdS with a higher reduction potential and the valence band (VB) of CuO with a higher oxidation potential under illumination, as expected for the S-scheme mechanism. Density-functional-theory calculations of the electron density difference (EDD) disclose an interfacial electric field oriented from CdS to CuO. This built-in field suppresses charge recombination and accelerates carrier migration, rationalizing the markedly enhanced PHE activity. This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-to-hydrogen conversion.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 1","pages":"Pages 1-13"},"PeriodicalIF":0.0,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957655","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 : 2026-01-01DOI: 10.1016/S1872-5813(25)60599-8
Xing LIU , Shaoqing GUO , Haitao CUI , Zhenrong LI , Xin LI , Lei WANG , Xingjie WU , Xiaoxiao WANG , Lijing YUAN , Liangfu ZHAO
KIT-5/Beta composite supports were synthesized using an in situ self-assembly hydrothermal method, and NiW/KIT-5/Beta catalysts were prepared by impregnation. A series of characterization techniques were utilized to evaluate the influence of varying hydrothermal synthesis temperatures on the physicochemical properties of both the KIT-5/Beta supports and the resulting catalysts. The catalytic performances of catalysts were evaluated under reaction conditions of 320 °C, 4 MPa H2 pressure, and a weight hourly space velocity (WHSV) of 4.8 h−1 for hydrodenitrogenation (HDN) of quinoline. The results indicated that the specific surface area and pore structure of the materials could be effectively regulated by adjusting the hydrothermal synthesis temperature, which in turn influenced the number of active sites on the catalyst. The NiW/KB-125 catalyst, synthesized at 125 °C, presented the highest quinoline HDN efficiency (96.8%), which can be attributed to its favorable pore channel structure, greater Brønsted acid number, higher degree of metal sulfidation (80.12%) and appropriate metal-support interaction (MSI).
采用原位自组装水热法制备了KIT-5/Beta复合载体，并采用浸渍法制备了NiW/KIT-5/Beta催化剂。利用一系列表征技术来评价不同水热合成温度对KIT-5/Beta载体和催化剂理化性质的影响。在320℃、4 MPa H2压力、4.8 h - 1的失重时空速（WHSV）条件下，考察了催化剂对喹啉加氢脱氮（HDN）的催化性能。结果表明，通过调节水热合成温度可以有效地调节材料的比表面积和孔结构，从而影响催化剂上活性位点的数量。在125℃条件下合成的NiW/KB-125催化剂的喹啉HDN效率最高（96.8%），这主要归功于其良好的孔道结构、较大的Brønsted酸数、较高的金属硫化度（80.12%）和适当的金属-载体相互作用（MSI）。
{"title":"Design and synthesis of KIT-5/Beta composites under varied hydrothermal temperatures and evaluation of their hydrodenitrogenation performance","authors":"Xing LIU , Shaoqing GUO , Haitao CUI , Zhenrong LI , Xin LI , Lei WANG , Xingjie WU , Xiaoxiao WANG , Lijing YUAN , Liangfu ZHAO","doi":"10.1016/S1872-5813(25)60599-8","DOIUrl":"10.1016/S1872-5813(25)60599-8","url":null,"abstract":"<div><div>KIT-5/Beta composite supports were synthesized using an <em>in situ</em> self-assembly hydrothermal method, and NiW/KIT-5/Beta catalysts were prepared by impregnation. A series of characterization techniques were utilized to evaluate the influence of varying hydrothermal synthesis temperatures on the physicochemical properties of both the KIT-5/Beta supports and the resulting catalysts. The catalytic performances of catalysts were evaluated under reaction conditions of 320 °C, 4 MPa H<sub>2</sub> pressure, and a weight hourly space velocity (WHSV) of 4.8 h<sup>−1</sup> for hydrodenitrogenation (HDN) of quinoline. The results indicated that the specific surface area and pore structure of the materials could be effectively regulated by adjusting the hydrothermal synthesis temperature, which in turn influenced the number of active sites on the catalyst. The NiW/KB-125 catalyst, synthesized at 125 °C, presented the highest quinoline HDN efficiency (96.8%), which can be attributed to its favorable pore channel structure, greater Brønsted acid number, higher degree of metal sulfidation (80.12%) and appropriate metal-support interaction (MSI).</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 1","pages":"Pages 1-12"},"PeriodicalIF":0.0,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957658","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 : 2026-01-01DOI: 10.1016/S1872-5813(25)60598-6
Jian NIU , Yuhang LI , Baofeng BAI , Chaolu WEN , Linbo LI , Huirong ZHANG , Shaoqing GUO
To elucidate the effect of calcite-regulated activated carbon (AC) structure on low-temperature denitrification performance of SCR catalysts, this work prepared a series of Mn-Ce/De-AC-xCaCO3 (x is the calcite content in coal) catalysts were prepared by the incipient wetness impregnation method, followed by acid washing to remove calcium-containing minerals. Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity. Specifically, NO conversion increased from 88.3% of Mn-Ce/De-AC to 91.7% of Mn-Ce/De-AC-1CaCO3 (210 °C). The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn4+ content and Ce4+/Ce3+ ratio, an abundance of chemisorbed oxygen and acidic sites, which could strengthen the SCR reaction pathways (richer NH3 activated species and bidentate nitrate active species). Therefore, NO removal is enhanced.
{"title":"Mechanism of enhancing NH3-SCR performance of Mn-Ce/AC catalyst by the structure regulation of activated carbon with calcite in coal","authors":"Jian NIU , Yuhang LI , Baofeng BAI , Chaolu WEN , Linbo LI , Huirong ZHANG , Shaoqing GUO","doi":"10.1016/S1872-5813(25)60598-6","DOIUrl":"10.1016/S1872-5813(25)60598-6","url":null,"abstract":"<div><div>To elucidate the effect of calcite-regulated activated carbon (AC) structure on low-temperature denitrification performance of SCR catalysts, this work prepared a series of Mn-Ce/De-AC-<em>x</em>CaCO<sub>3</sub> (<em>x</em> is the calcite content in coal) catalysts were prepared by the incipient wetness impregnation method, followed by acid washing to remove calcium-containing minerals. Comprehensive characterization and low-temperature denitrification tests revealed that calcite-induced structural modulation of coal-derived AC significantly enhances catalytic activity. Specifically, NO conversion increased from 88.3% of Mn-Ce/De-AC to 91.7% of Mn-Ce/De-AC-1CaCO<sub>3</sub> (210 °C). The improved SCR denitrification activity results from the enhancement of physicochemical properties including higher Mn<sup>4+</sup> content and Ce<sup>4+</sup>/Ce<sup>3+</sup> ratio, an abundance of chemisorbed oxygen and acidic sites, which could strengthen the SCR reaction pathways (richer NH<sub>3</sub> activated species and bidentate nitrate active species). Therefore, NO removal is enhanced.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 1","pages":"Pages 1-11"},"PeriodicalIF":0.0,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957659","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 : 2026-01-01DOI: 10.1016/S1872-5813(25)60593-7
Yuanyuan GE , Yuzhe WANG , Guozhong XU , Yaming ZHU , Xia YUAN , Guimei SHI , Xiangyun ZHONG
The development of materials with excellent microwave absorption (MWA) and electromagnetic interference (EMI) shielding performances has currently received attention. Herein, mesophase pitch-based carbon foam (MPCF) with 3D interconnected pore structure was prepared through the high pressure pyrolysis of mesophase coal tar pitch. It is found that the 3D interconnected cellular pores of MPCF facilitate multiple reflections of electromagnetic waves, which results in the minimum reflection loss (RLmin) value of MPCF reaches −37.84 dB with the effective absorption bandwidth (EAB) of 5.44 GHz at a thickness of 2.70 mm, and the total average electromagnetic shielding effectiveness (SET) under 3.00 mm thickness achieves 26.52 dB in X-band. Subsequently, MPCF is activated by KOH to obtain activated carbon foam (A-MPCF). The average SET of A-MPCF achieves 103.00 dB for abundant nanopores on the pore cell walls, which leads to a transition from the multiple reflections of electromagnetic waves on the walls to diffuse reflection. Unfortunately, the reflection coefficient (R) of A-MPCF increases from 0.78 to 0.90. To reduce the R value, Fe3O4/A-MPCF was fabricated via the in situ growth of nano Fe3O4 on A-MPCF. Consequently, the R value of Fe3O4/A-MPCF was reduced from 0.90 to 0.74, whereas the MWA performance was only slightly decreased. This work proposes a simple strategy for simultaneously adjusting MWA and EMI shielding performances of materials.
{"title":"Preparation and tailoring electromagnetic shielding and microwave absorbing performance of Fe3O4 modified activated carbon foam based on mesophase coal pitch pyrolysis foaming","authors":"Yuanyuan GE , Yuzhe WANG , Guozhong XU , Yaming ZHU , Xia YUAN , Guimei SHI , Xiangyun ZHONG","doi":"10.1016/S1872-5813(25)60593-7","DOIUrl":"10.1016/S1872-5813(25)60593-7","url":null,"abstract":"<div><div>The development of materials with excellent microwave absorption (MWA) and electromagnetic interference (EMI) shielding performances has currently received attention. Herein, mesophase pitch-based carbon foam (MPCF) with 3D interconnected pore structure was prepared through the high pressure pyrolysis of mesophase coal tar pitch. It is found that the 3D interconnected cellular pores of MPCF facilitate multiple reflections of electromagnetic waves, which results in the minimum reflection loss (<em>RL</em><sub>min</sub>) value of MPCF reaches −37.84 dB with the effective absorption bandwidth (<em>EAB</em>) of 5.44 GHz at a thickness of 2.70 mm, and the total average electromagnetic shielding effectiveness (<em>SE</em><sub>T</sub>) under 3.00 mm thickness achieves 26.52 dB in X-band. Subsequently, MPCF is activated by KOH to obtain activated carbon foam (A-MPCF). The average SE<sub>T</sub> of A-MPCF achieves 103.00 dB for abundant nanopores on the pore cell walls, which leads to a transition from the multiple reflections of electromagnetic waves on the walls to diffuse reflection. Unfortunately, the reflection coefficient (<em>R</em>) of A-MPCF increases from 0.78 to 0.90. To reduce the <em>R</em> value, Fe<sub>3</sub>O<sub>4</sub>/A-MPCF was fabricated via the <em>in situ</em> growth of nano Fe<sub>3</sub>O<sub>4</sub> on A-MPCF. Consequently, the <em>R</em> value of Fe<sub>3</sub>O<sub>4</sub>/A-MPCF was reduced from 0.90 to 0.74, whereas the MWA performance was only slightly decreased. This work proposes a simple strategy for simultaneously adjusting MWA and EMI shielding performances of materials.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 1","pages":"Pages 1-15"},"PeriodicalIF":0.0,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957681","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}
Needle coke, a high-performance artificial carbon material, requires precise composition control of its raw materials as this critically determines the structural characteristics and performance of the final product. In this study, needle coke samples were prepared from coal direct liquefaction pitch (CDLP) and waste engine oil (WEO) through component optimization and a co-carbonization process. The microstructure and properties were investigated using the following characterization techniques: Fourier Transform Infrared Spectroscopy (FT-IR), Polarized Light Microscopy (PLM), Scanning Electron Microscopy (SEM), X-ray Diffraction (XRD), Raman Spectroscopy, Thermogravimetric Analysis (TGA), Micro-Strength (MS) and Powder Resistivity (PR). The co-carbonization mechanism of CDLP and WEO was systematically investigated. The results indicated that the incorporation of WEO significantly reduced the viscosity of the co-carbonization system, and its abundant aliphatic structures provided alkyl radicals and active sites. The synergistic interaction of aromatic components between the CDLP and WEO effectively promoted the growth and order accumulation of aromatic carbon layers. When 50% WEO was introduced, the prepared needle coke exhibited an excellent microstructure and properties. The fibrous and leaflet structure content reached 76.2%, the ideal graphite lattice content reached 89.7%. These results demonstrated remarkable oxidation resistance and electrical conductivity, with a powder resistivity of 605.1 mΩ·mm. This work establishes a process with cost advantages for the production of needle coke.
{"title":"Preparation and structure evolution of coal-based needle coke by co-carbonization of coal direct liquefaction pitch and waste engine oil","authors":"Yuzhu ZHANG , Yuan QI , Yaming ZHU , Junxia CHENG , Xuefei ZHAO","doi":"10.1016/S1872-5813(25)60591-3","DOIUrl":"10.1016/S1872-5813(25)60591-3","url":null,"abstract":"<div><div>Needle coke, a high-performance artificial carbon material, requires precise composition control of its raw materials as this critically determines the structural characteristics and performance of the final product. In this study, needle coke samples were prepared from coal direct liquefaction pitch (CDLP) and waste engine oil (WEO) through component optimization and a co-carbonization process. The microstructure and properties were investigated using the following characterization techniques: Fourier Transform Infrared Spectroscopy (FT-IR), Polarized Light Microscopy (PLM), Scanning Electron Microscopy (SEM), X-ray Diffraction (XRD), Raman Spectroscopy, Thermogravimetric Analysis (TGA), Micro-Strength (MS) and Powder Resistivity (PR). The co-carbonization mechanism of CDLP and WEO was systematically investigated. The results indicated that the incorporation of WEO significantly reduced the viscosity of the co-carbonization system, and its abundant aliphatic structures provided alkyl radicals and active sites. The synergistic interaction of aromatic components between the CDLP and WEO effectively promoted the growth and order accumulation of aromatic carbon layers. When 50% WEO was introduced, the prepared needle coke exhibited an excellent microstructure and properties. The fibrous and leaflet structure content reached 76.2%, the ideal graphite lattice content reached 89.7%. These results demonstrated remarkable oxidation resistance and electrical conductivity, with a powder resistivity of 605.1 mΩ·mm. This work establishes a process with cost advantages for the production of needle coke.</div></div>","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 1","pages":"Pages 1-13"},"PeriodicalIF":0.0,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957660","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 : 2026-01-01DOI: 10.1016/S1872-5813(25)60588-3
Zhifu YU , Lei JIANG , Mingbo WU
<div><div>Against the backdrop of escalating global climate change and energy crises, the resource utilization of carbon dioxide (CO<sub>2</sub>), a major greenhouse gas, has become a crucial pathway for achieving carbon peaking and carbon neutrality goals. The hydrogenation of CO<sub>2</sub> to methanol not only enables carbon sequestration and recycling, but also provides a route to produce high value-added fuels and basic chemical feedstocks, holding significant environmental and economic potential. However, this conversion process is thermodynamically and kinetically limited, and traditional catalyst systems (e.g., Cu/ZnO/Al<sub>2</sub>O<sub>3</sub>) exhibit inadequate activity, selectivity, and stability under mild conditions. Therefore, the development of novel high-performance catalysts with precisely tunable structures and functionalities is imperative. Metal-organic frameworks (MOFs), as crystalline porous materials with high surface area, tunable pore structures, and diverse metal-ligand compositions, have the great potential in CO<sub>2</sub> hydrogenation catalysis. Their structural design flexibility allows for the construction of well-dispersed active sites, tailored electronic environments, and enhanced metal-support interactions. This review systematically summarizes the recent advances in MOF-based and MOF-derived catalysts for CO<sub>2</sub> hydrogenation to methanol, focusing on four design strategies: (1) spatial confinement and <em>in situ</em> construction, (2) defect engineering and ion-exchange, (3) bimetallic synergy and hybrid structure design, and (4) MOF-derived nanomaterial synthesis. These approaches significantly improve CO<sub>2</sub> conversion and methanol selectivity by optimizing metal dispersion, interfacial structures, and reaction pathways. The reaction mechanism is further explored by focusing on the three main reaction pathways: the formate pathway (HCOO*), the RWGS (Reverse Water Gas Shift reaction) + CO* hydrogenation pathway, and the trans-COOH pathway. <em>In situ</em> spectroscopic studies and density functional theory (DFT) calculations elucidate the formation and transformation of key intermediates, as well as the roles of active sites, metal-support interfaces, oxygen vacancies, and promoters. Additionally, representative catalytic performance data for MOF-based systems are compiled and compared, demonstrating their advantages over traditional catalysts in terms of CO<sub>2</sub> conversion, methanol selectivity, and space-time yield. Future perspectives for MOF-based CO<sub>2</sub> hydrogenation catalysts will prioritize two main directions: structural design and mechanistic understanding. The precise construction of active sites through multi-metallic synergy, defect engineering, and interfacial electronic modulation should be made to enhance catalyst selectivity and stability. In addition, advanced <em>in situ</em> characterization techniques combined with theoretical modeling are essential to u
在全球气候变化和能源危机日益加剧的背景下，二氧化碳作为主要温室气体的资源利用已成为实现碳峰值和碳中和目标的重要途径。二氧化碳加氢制甲醇不仅可以实现碳固存和循环利用，而且还提供了一条生产高附加值燃料和基础化学原料的途径，具有重大的环境和经济潜力。然而，这种转化过程受到热力学和动力学的限制，传统的催化剂体系（例如Cu/ZnO/Al2O3）在温和条件下表现出不足的活性、选择性和稳定性。因此，开发具有精确可调结构和功能的新型高性能催化剂势在必行。金属有机骨架（MOFs）作为具有高比表面积、可调孔结构和多种金属配体组成的晶体多孔材料，在CO2加氢催化中具有巨大的潜力。它们的结构设计灵活性允许构建分散良好的活性位点、定制的电子环境和增强的金属支撑相互作用。本文系统总结了近年来基于mof和衍生mof的CO2加氢制甲醇催化剂的研究进展，重点介绍了四种设计策略：(1)空间约束和原位构建，(2)缺陷工程和离子交换，(3)双金属协同和杂化结构设计，(4)mof衍生纳米材料合成。这些方法通过优化金属分散、界面结构和反应途径，显著提高了CO2转化率和甲醇选择性。进一步探讨了反应机理，重点研究了甲酸酯途径（HCOO*）、RWGS (Reverse Water Gas Shift reaction) + CO*加氢途径和反式cooh途径三种主要反应途径。原位光谱研究和密度泛函理论（DFT）计算阐明了关键中间体的形成和转变，以及活性位点、金属支撑界面、氧空位和启动子的作用。此外，对mof系统的代表性催化性能数据进行了汇编和比较，证明了它们在CO2转化率、甲醇选择性和时空产率方面优于传统催化剂。未来基于mof的CO2加氢催化剂的研究将优先考虑两个主要方向：结构设计和机理理解。通过多金属协同作用、缺陷工程和界面电子调制等方法精确构建活性位点，提高催化剂的选择性和稳定性。此外，先进的原位表征技术与理论建模相结合对于揭示详细的反应机理和中间行为至关重要，从而指导合理的催化剂设计。此外，为了实现工业应用，必须解决与热/水热稳定性，催化剂可回收性和成本效益大规模合成相关的挑战。开发绿色、可扩展的制备方法，并将MOF催化剂集成到实际反应系统（例如流动反应器）中，对于弥合实验室研究和商业部署之间的差距至关重要。最终，多尺度结构性能优化和催化系统集成对于加速基于mof的二氧化碳制甲醇技术的产业化至关重要。
{"title":"Progress in MOF-based catalyst design and reaction mechanisms for CO2 hydrogenation to methanol","authors":"Zhifu YU , Lei JIANG , Mingbo WU","doi":"10.1016/S1872-5813(25)60588-3","DOIUrl":"10.1016/S1872-5813(25)60588-3","url":null,"abstract":"<div><div>Against the backdrop of escalating global climate change and energy crises, the resource utilization of carbon dioxide (CO<sub>2</sub>), a major greenhouse gas, has become a crucial pathway for achieving carbon peaking and carbon neutrality goals. The hydrogenation of CO<sub>2</sub> to methanol not only enables carbon sequestration and recycling, but also provides a route to produce high value-added fuels and basic chemical feedstocks, holding significant environmental and economic potential. However, this conversion process is thermodynamically and kinetically limited, and traditional catalyst systems (e.g., Cu/ZnO/Al<sub>2</sub>O<sub>3</sub>) exhibit inadequate activity, selectivity, and stability under mild conditions. Therefore, the development of novel high-performance catalysts with precisely tunable structures and functionalities is imperative. Metal-organic frameworks (MOFs), as crystalline porous materials with high surface area, tunable pore structures, and diverse metal-ligand compositions, have the great potential in CO<sub>2</sub> hydrogenation catalysis. Their structural design flexibility allows for the construction of well-dispersed active sites, tailored electronic environments, and enhanced metal-support interactions. This review systematically summarizes the recent advances in MOF-based and MOF-derived catalysts for CO<sub>2</sub> hydrogenation to methanol, focusing on four design strategies: (1) spatial confinement and <em>in situ</em> construction, (2) defect engineering and ion-exchange, (3) bimetallic synergy and hybrid structure design, and (4) MOF-derived nanomaterial synthesis. These approaches significantly improve CO<sub>2</sub> conversion and methanol selectivity by optimizing metal dispersion, interfacial structures, and reaction pathways. The reaction mechanism is further explored by focusing on the three main reaction pathways: the formate pathway (HCOO*), the RWGS (Reverse Water Gas Shift reaction) + CO* hydrogenation pathway, and the trans-COOH pathway. <em>In situ</em> spectroscopic studies and density functional theory (DFT) calculations elucidate the formation and transformation of key intermediates, as well as the roles of active sites, metal-support interfaces, oxygen vacancies, and promoters. Additionally, representative catalytic performance data for MOF-based systems are compiled and compared, demonstrating their advantages over traditional catalysts in terms of CO<sub>2</sub> conversion, methanol selectivity, and space-time yield. Future perspectives for MOF-based CO<sub>2</sub> hydrogenation catalysts will prioritize two main directions: structural design and mechanistic understanding. The precise construction of active sites through multi-metallic synergy, defect engineering, and interfacial electronic modulation should be made to enhance catalyst selectivity and stability. In addition, advanced <em>in situ</em> characterization techniques combined with theoretical modeling are essential to u","PeriodicalId":15956,"journal":{"name":"燃料化学学报","volume":"54 1","pages":"Pages 1-17"},"PeriodicalIF":0.0,"publicationDate":"2026-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957682","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}
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