Catalysis Letters最新文献_第7页

Chiral Phosphine-Aminophosphine Ligands for Copper-Catalyzed Asymmetric Hydrogenation 铜催化不对称氢化的手性膦-氨基膦配体

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-03-09 DOI: 10.1007/s10562-026-05344-1

Zita Szabó, Zsófia Császár, Margit Kovács, József Bakos, Gergely Farkas

{"title":"Chiral Phosphine-Aminophosphine Ligands for Copper-Catalyzed Asymmetric Hydrogenation","authors":"Zita Szabó, Zsófia Császár, Margit Kovács, József Bakos, Gergely Farkas","doi":"10.1007/s10562-026-05344-1","DOIUrl":"10.1007/s10562-026-05344-1","url":null,"abstract":"<div><p>New chiral bidentate phosphine-aminophosphine ligands based on a pentane-2,4-diyl backbone, with the general formula Ph<sub>2</sub>PCH(CH<sub>3</sub>)CH<sub>2</sub>CH(CH<sub>3</sub>)N(R<sup>1</sup>)PR<sup>2</sup><sub>2</sub> (R<sup>1</sup> = Me, Et, <i>n</i>Pr, <i>n</i>Bu, <i>i</i>Pr; R<sup>2</sup> = Ph, Cy), have been developed and applied in the copper-catalyzed asymmetric hydrogenation of simple ketones. The addition of achiral monodentate phosphines as co-ligands significantly enhanced both catalytic turnover and enantioselectivity. It was observed that the steric properties of the ligands predominantly influence catalytic activity and enantioinduction, whereas their electronic characteristics play a secondary role. Comprehensive screening of reaction conditions, including variation of the metal source and careful selection of both chiral and achiral ligands with appropriately tuned stereochemistry, enabled the hydrogenation to proceed with low catalyst loadings (0.5 mol%) while maintaining high yields and enantioselectivities (up to 92% <i>ee</i>) across a broad substrate scope. Based on experimental findings and relevant literature precedents, a mechanistic proposal is presented to explain the observed reactivity trends.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div><div><p>Graphical Abstract</p></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10562-026-05344-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147440917","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pd-Catalyzed Aminocarbonylation of Aryldiazonium Tetrafluoroborate Salts with Ammonia Surrogate to Access Primary Amides Under Ligand and Base-Free Conditions 在配体和无碱条件下，用氨替代物催化芳基重氮四氟硼酸盐氨基羰基化制备伯胺

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-03-07 DOI: 10.1007/s10562-026-05349-w

Bharati Mourya, Shankar B. Chaudhari, Sandip T. Gadge, Bhalchandra M. Bhanage

{"title":"Pd-Catalyzed Aminocarbonylation of Aryldiazonium Tetrafluoroborate Salts with Ammonia Surrogate to Access Primary Amides Under Ligand and Base-Free Conditions","authors":"Bharati Mourya, Shankar B. Chaudhari, Sandip T. Gadge, Bhalchandra M. Bhanage","doi":"10.1007/s10562-026-05349-w","DOIUrl":"10.1007/s10562-026-05349-w","url":null,"abstract":"<div><p>A sustainable, new, and efficient protocol has been developed, which provides a mild route to primary amides via Pd-catalyzed aminocarbonylation of aryldiazonium tetrafluoroborate salts with an ammonia surrogate under ligand and base-free conditions. The employment of readily available aryldiazonium salts, derived from inexpensive anilines, as aryl sources renders this transformation both practically and economically. Characteristically, this study reports the first ligand and base-free aminocarbonylation employing an ammonia surrogate with diazonium salts. The methodology demonstrates broad substrate compatibility, tolerating diverse functional groups and delivering the desired primary amides in good to excellent yields. This operationally simple and environmentally benign approach eliminates the need for gaseous ammonia and external ligand and bases, offering a mild, atom-economical, and efficient strategy for primary amide synthesis.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div><div><p>In this protocol, a novel, sustainable, simple and efficient palladium-catalyzed protocol has been developed for the access of primary amides via aminocarbonylation of aryldiazonium tetrafluoroborate salts with an ammonia surrogate, providing a mild route to primary amides under ligand and base-free conditions.</p></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147362950","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Production of Hydrogen Gas via Pt/C Catalyzed Decomposition of Formic Acid Pt/C催化甲酸分解制氢研究

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-03-07 DOI: 10.1007/s10562-026-05336-1

Tayyaba Batool, Mansor Hussain, Muhammad Saeed, Nadia Akram, Muhammad Usman, Javeria Hassan, Dania Arif

{"title":"Production of Hydrogen Gas via Pt/C Catalyzed Decomposition of Formic Acid","authors":"Tayyaba Batool, Mansor Hussain, Muhammad Saeed, Nadia Akram, Muhammad Usman, Javeria Hassan, Dania Arif","doi":"10.1007/s10562-026-05336-1","DOIUrl":"10.1007/s10562-026-05336-1","url":null,"abstract":"<div><p>The pollution-free combustion and high energy density of hydrogen gas make it a suitable and clean energy carrier. However, its sustainable, safe, and efficient production and transportation are the major challenges that limit the practical applications of hydrogen as a source of energy. In this study, hydrogen gas was produced via Platinum supported on carbon (Pt/C) catalyzed decomposition of formic acid, a liquid hydrogen carrier. Various Pt/C catalysts loaded with 1, 4, 6, 8, and 10% Pt were prepared and utilized as catalysts for the decomposition of formic acid. The 6% Pt/C was found as effective catalyst, achieving maximum gas production within the shortest reaction time under mild conditions (60 °C, 0.2 M formic acid, 0.04 g catalyst) in this study. The progress of the reaction was monitored by measuring the total volume of gas produced by the water displacement method. Kinetic analysis based on a Langmuir–Hinshelwood model yielded an apparent rate constant of 0.2136 min<sup>− 1</sup>, indicating efficient surface-mediated catalysis. The energy of activation was calculated as 81.1 kJ/mol. It was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDX), and scanning electron microscopy (SEM). The results demonstrate that optimized Pt/C catalysts enable efficient, low-temperature hydrogen generation from formic acid, highlighting the potential of this system as a viable route for hydrogen storage and on-demand hydrogen production.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div><div><p>Production of Hydrogen by catalytic decomposition of formic acid</p></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147362952","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Energy-Efficient Microwave-Assisted Benzene Oxidation over MnOx/K-ZSM-5 Zeolite in Intermittent Heating Mode 间歇加热模式下MnOx/K-ZSM-5沸石上高效微波辅助苯氧化

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-03-07 DOI: 10.1007/s10562-026-05322-7

Liyun Zhang, Hisahiro Einaga

{"title":"Energy-Efficient Microwave-Assisted Benzene Oxidation over MnOx/K-ZSM-5 Zeolite in Intermittent Heating Mode","authors":"Liyun Zhang, Hisahiro Einaga","doi":"10.1007/s10562-026-05322-7","DOIUrl":"10.1007/s10562-026-05322-7","url":null,"abstract":"<div><p>Catalytic oxidation of volatile organic compounds (VOCs) in intermittent heating mode is generally energy efficient. However, the application of intermittent heating, especially with microwave (MW) assistance, remains a severe challenge due to its requirements on the dielectric and VOCs adsorption properties of the catalyst. Here, potassium ion exchanged ZSM-5 (KZ-23) with the best MW heating performance was synthesized and used as the support, and three Mn modified KZ-23 catalysts with different Mn loadings were prepared by a simple impregnation method. 20Mn/KZ-23 (loading 20 wt% Mn) shows excellent catalytic activity in MW-assisted catalytic oxidation of benzene due to its relatively high content of Mn<sub>2</sub>O<sub>3</sub> phase and low average oxidation state of Mn. Moreover, the adsorption capacity of 20Mn/KZ-23 for benzene and its rapid response to MW enables it to exhibit satisfactory performance in intermittent heating mode. The average benzene conversion over the catalyst is 57.1%, while its energy consumption is only 12.3% of that in continuous heating mode with a similar conversion. This work provides a guidance for the rational design of energy-efficient heating modes in MW-assisted VOC catalytic oxidation.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147362953","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Molecularly Imprinted-g-C3N5 for Photocatalytic Oxidation of d-glucose 分子印迹g- c3n5光催化氧化d-葡萄糖

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-03-07 DOI: 10.1007/s10562-026-05348-x

Zhanqiu Tang, Yuqing Fu, Xinyi Feng, Zhenglong Wu, Weidong Qin

{"title":"Molecularly Imprinted-g-C3N5 for Photocatalytic Oxidation of d-glucose","authors":"Zhanqiu Tang, Yuqing Fu, Xinyi Feng, Zhenglong Wu, Weidong Qin","doi":"10.1007/s10562-026-05348-x","DOIUrl":"10.1007/s10562-026-05348-x","url":null,"abstract":"<div><p>Enantioselective catalytic oxidation of <span>d</span>-glucose has been extensively applied in food, pharmaceutical, and chemical industries. In this work, a nitrogen-rich graphitic carbon nitride (<i>g-</i>C<sub>3</sub>N<sub>5</sub>) was synthesized through the pyrolysis of 3-amino-1,2,4-triazole. This material exhibited a reduced band gap, enhanced electrical conductivity, and superior photocatalytic performance compared to graphitic C<sub>3</sub>N<sub>4</sub> (<i>g-</i>C<sub>3</sub>N<sub>4</sub>), facilitating more efficient photocatalytic oxidation of glucose with higher yield. The surface of <i>g-</i>C<sub>3</sub>N<sub>5</sub> was subsequently capped with a molecularly imprinted polymer (MIP) layer by employing <span>d</span>-glucose as the template molecule, and 4-vinylphenylboronic acid as the functional monomer. The resulting <i>g-</i>C<sub>3</sub>N<sub>5</sub>-MIPs demonstrated the ability to selectively photocatalyze the oxidation of <span>d</span>-glucose, producing <span>d</span>-glu acid and H<sub>2</sub>O<sub>2</sub>. Notably, the relative selectivity coefficient for <span>d</span>-glucose over <span>l</span>-glucose increased by a factor of 8.79 compared to the non-imprinted <i>g-</i>C<sub>3</sub>N<sub>5</sub>. This work presents an effective approach for synthesizing advanced g-C<sub>3</sub>N<sub>5</sub>-MIP-based photocatalysts, and highlights their potential for highly enantioselective aerobic oxidation of <span>d</span>-glucose.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147362954","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Efficient Preparation of Black Phosphorus Enabled by Sn24P19.3I8/Graphite Catalyst with Enhanced Thermal Conductivity Sn24P19.3I8/石墨催化剂增强导热性能制备黑磷

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-03-07 DOI: 10.1007/s10562-026-05342-3

Tun Nile, Hao Sun, Tingting Xu, Yu Yang, Caimei He, Wen Chen, Peichao Lian

{"title":"Efficient Preparation of Black Phosphorus Enabled by Sn24P19.3I8/Graphite Catalyst with Enhanced Thermal Conductivity","authors":"Tun Nile, Hao Sun, Tingting Xu, Yu Yang, Caimei He, Wen Chen, Peichao Lian","doi":"10.1007/s10562-026-05342-3","DOIUrl":"10.1007/s10562-026-05342-3","url":null,"abstract":"<div><p>The mineralization method boasts advantages including high product purity, controllable crystal structure and good reproducibility, making it a promising approach for the preparation of black phosphorus (BP). However, the employed Sn<sub>24</sub>P<sub>19.3</sub>I<sub>8</sub> catalyst suffers from pronounced sintering during the preparation process, which severely compromises its catalytic activity and cycle period. The yield (56.0%) was significantly low after two cycles of BP preparation by using Sn<sub>24</sub>P<sub>19.3</sub>I<sub>8</sub>. Herein, intrinsically low thermal conductivity (1.73 W m<sup>−1</sup> K<sup>−1</sup>) was demonstrated to the decreased catalytic performance of Sn<sub>24</sub>P<sub>19.3</sub>I<sub>8</sub> catalyst. To overcome this issue, graphite was integrated with Sn<sub>24</sub>P<sub>19.3</sub>I<sub>8</sub> (Sn<sub>24</sub>P<sub>19.3</sub>I<sub>8</sub>/Gra) for improving the thermal conductivity (15.75 W m<sup>−1</sup> K<sup>−1</sup>), which effectively alleviated the issue of local heat accumulation and therefore overcame sintering of Sn<sub>24</sub>P<sub>19.3</sub>I<sub>8</sub>. As expected, an exceptionally high yield of 83.3% was achieved even after nine cycles of BP preparation based on the Sn<sub>24</sub>P<sub>19.3</sub>I<sub>8</sub>/Gra composite catalyst, highlighting the catalytic robustness. This work provided a feasible production of high-quality BP, paving the way for its broad industrial application.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147362951","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Construction of Ni-GaOx Sites on Hierarchical Porous SBA-15 Support for Propane Dehydrogenation 分层多孔SBA-15丙烷脱氢载体上Ni-GaOx位点的构建

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-03-04 DOI: 10.1007/s10562-026-05319-2

Huibo Qin, Zhenkun Zhang, Jian Shen, Zebing Bao, Ziming Huang, Yinjie Liu, Linhai Duan, Xiuhong Meng, Leiming Tao

{"title":"Construction of Ni-GaOx Sites on Hierarchical Porous SBA-15 Support for Propane Dehydrogenation","authors":"Huibo Qin, Zhenkun Zhang, Jian Shen, Zebing Bao, Ziming Huang, Yinjie Liu, Linhai Duan, Xiuhong Meng, Leiming Tao","doi":"10.1007/s10562-026-05319-2","DOIUrl":"10.1007/s10562-026-05319-2","url":null,"abstract":"<div><p>Propane dehydrogenation (PDH) to propylene is a key industrial process, and the development of high-performance non-precious metal catalysts remains a significant challenge. In this work, hierarchical porous SBA-15 was prepared as a catalyst support, and bimetallic Ni-GaO<sub>x</sub> species were loaded onto SBA-15 surface via incipient wetness impregnation to fabricate related catalysts. The catalyst structure and PDH performance were systematically investigated using a combination of characterization techniques, with catalytic activity evaluated in a fixed-bed reactor. Results showed that the 20Ni/SBA-15 catalyst (single Ni-loaded) exhibited a propane conversion of ~ 10%, but no propylene was detected due to severe non-selective side reactions. With increasing Ga<sub>2</sub>O<sub>3</sub> content, propylene yield gradually increased, and the 20Ni<sub>1</sub>Ga<sub>2</sub>/SBA-15 catalyst achieved an excellent propylene yield with sustained high selectivity. Methane and ethylene were generated as by-products during the reaction. Eventually, thermogravimetric analysis was performed on both fresh and spent catalysts, which confirmed the formation of graphitic coke deposits. This work provides a feasible strategy for designing and optimizing Ni-based catalysts via Ga<sub>2</sub>O<sub>3</sub> modification, which is expected to guide the development of high-selectivity and anti-coking dehydrogenation catalysts.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147363217","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Tailoring the Optoelectronics Properties of ZnO Nanostructures Through Metal Doping for Efficient Photocatalysis and Photovoltaic Application 通过金属掺杂调整ZnO纳米结构的光电性能用于高效光催化和光伏应用

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-03-01 DOI: 10.1007/s10562-026-05332-5

Zain ul Abideen, Salma Shad, Muhammad Usman Farooq, Uswa Hassan, Aliya Ibrar, Muzaffar Iqbal

{"title":"Tailoring the Optoelectronics Properties of ZnO Nanostructures Through Metal Doping for Efficient Photocatalysis and Photovoltaic Application","authors":"Zain ul Abideen, Salma Shad, Muhammad Usman Farooq, Uswa Hassan, Aliya Ibrar, Muzaffar Iqbal","doi":"10.1007/s10562-026-05332-5","DOIUrl":"10.1007/s10562-026-05332-5","url":null,"abstract":"<div><p>Herein, zirconium-doped ZnO nanostructures were prepared by a hydrothermal approach with different concentrations of dopants (2%, 4%, and 6%). The as-synthesized materials were characterized through UV-Visible spectroscopy, X-ray diffraction (XRD), Photoluminescence (PL) spectroscopy, scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), and elemental mapping. The UV-Visible results showed that Zr doping enhanced the absorption range due to the introduction of additional Fermi levels above the valence band of pure ZnO, which enabled the absorption of photons with lower energy. The PL study revealed that charge separation efficiency is enhanced, and recombination processes are deterred by doping in pure ZnO. XRD analysis indicated that the synthesized materials possess a high degree of crystallinity, and the successful incorporation of Zr<sup>4+</sup> ions onto the ZnO crystal lattice was confirmed. EDX and elemental mapping results indicate the presence of backbone elements (Zn, O, and Zr) and a uniform distribution of elements in the as-synthesized samples. The as-prepared nanostructures were employed as photoanodes in dye-sensitized solar cells (DSSCs) and photocatalytic reduction of salicylic acid in wastewater. Among the samples, the 6% Zr doped ZnO showed excellent performance in both photovoltaic and photocatalytic applications. This high efficiency is attributed to high charge separation efficiency and large light absorption ability. This synthesis approach demonstrated the considerable potential in enhancing both the solar energy conversion efficiency of DSSCs and the photocatalytic potential of pure ZnO nanorods (NRs).</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147335729","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Photothermal Enhanced Charge Transfer and Protonation for Selective Photocatalytic CO2 Conversion to CH4 选择性光催化CO2转化为CH4的光热增强电荷转移和质子化

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-02-23 DOI: 10.1007/s10562-026-05323-6

Zhihong Wang, Jun He, Zhongkai Xie, Min Chen, Weidong Shi

{"title":"Photothermal Enhanced Charge Transfer and Protonation for Selective Photocatalytic CO2 Conversion to CH4","authors":"Zhihong Wang, Jun He, Zhongkai Xie, Min Chen, Weidong Shi","doi":"10.1007/s10562-026-05323-6","DOIUrl":"10.1007/s10562-026-05323-6","url":null,"abstract":"<div><p>Photocatalytic reduction of CO<sub>2</sub> to CH<sub>4</sub> on TiO<sub>2</sub> remains a major challenge due to the complex multiple electron-proton coupling process. Notably, photothermal catalysis by synergistically promoting photogenerated charge separation and thermodynamic modulation has emerged as a promising strategy to promote the selective CH<sub>4</sub> production, while the special influence of photo-to-thermal effect on such process is still indistinct. In this work, TiO<sub>2</sub> exhibits an outstanding CH<sub>4</sub> production rate of 29.79 µmol·g<sup>− 1</sup>·h<sup>− 1</sup> with hugely increased CH<sub>4</sub> selectivity of 87.0% only rely on the optimization of reaction conditions (light intensity dominated photo-to-thermal effects). Combined in situ DRIFTS, electrochemical characterization, and DFT theoretical simulations indicate that photothermal heating not only accelerate the charge transfer but also lowers the energy barrier for CO<sub>2</sub> protonation, promoting formation of the multiple electron-proton coupling CH<sub>4</sub>. This work demonstrates that photothermal synergy not only enhances catalytic activity but also enables precise control of CH<sub>4</sub> product selectivity through heat-mediated modulation of intermediate transformations. These findings provide a novel strategy for the highly efficient and selective photocatalytic conversion of CO<sub>2</sub> to CH<sub>4</sub> and have positive implications for advancing sustainable carbon utilization.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147341493","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Surface Spin Effect in Chemisorption and Catalysis: Computational Robustness 化学吸附和催化中的表面自旋效应：计算鲁棒性

IF 2.3 4区化学

Catalysis Letters Pub Date : 2026-02-23 DOI: 10.1007/s10562-026-05334-3

Luis A. Cipriano, Oliver Christensen, Benjamin Grimm, Jens K. Nørskov

{"title":"Surface Spin Effect in Chemisorption and Catalysis: Computational Robustness","authors":"Luis A. Cipriano, Oliver Christensen, Benjamin Grimm, Jens K. Nørskov","doi":"10.1007/s10562-026-05334-3","DOIUrl":"10.1007/s10562-026-05334-3","url":null,"abstract":"<div><p>In this work, we show that the spin effect in chemisorption and catalysis is independent of the chosen exchange-correlation functional. Density functional theory simulations were performed to calculate the adsorption energies of carbon monoxide, hydrogen, and oxygen on a cobalt cluster and a cobalt surface. Eight commonly used exchange-correlation functionals were evaluated: three generalized gradient approximation (GGA) functionals (BEEF-vdW, PBE and RPBE), two meta-GGA functionals (RTPSS and r²SCAN), and three hybrid functionals (PBE0, HSE03, HSE06). All functionals were applied to the cluster model, while six were used for the surface. Across all levels of theory, non-spin-polarized ground states exhibit stronger binding than spin-polarized solutions. The adsorption energy difference scales with the local average spin moment, with smaller energy differences corresponding to lower spin moments, providing direct evidence that adsorption energies decrease as the spin moment decreases. The consistency of this trend across all tested functionals highlights the generality and robustness of the spin effect in chemisorption and its impact on catalysis.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"156 4","pages":""},"PeriodicalIF":2.3,"publicationDate":"2026-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10562-026-05334-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147341144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0