Journal of Catalysis最新文献_第9页

Effective hollow Rh@H-S-1 catalyst for hydroformylation of 1-hexene 用于 1-己烯加氢甲酰化的高效中空 Rh@H-S-1 催化剂

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-21 DOI: 10.1016/j.jcat.2024.115770

Gongcheng Sun, Subing Fan, Junmin Lv, Tiansheng Zhao

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Altering preferential product selectivity in electrocatalytic CO2 reduction over fluorine-modified CuIn bimetallic materials 改变氟改性 CuIn 双金属材料在电催化二氧化碳还原过程中的优先产物选择性

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-20 DOI: 10.1016/j.jcat.2024.115768

Lin Gu, Abhishek Dutta Chowdhury

{"title":"Altering preferential product selectivity in electrocatalytic CO2 reduction over fluorine-modified CuIn bimetallic materials","authors":"Lin Gu, Abhishek Dutta Chowdhury","doi":"10.1016/j.jcat.2024.115768","DOIUrl":"10.1016/j.jcat.2024.115768","url":null,"abstract":"<div><div>Integrating carbon dioxide (CO<sub>2</sub>)-derived renewable technologies into the petrochemical industry presents a promising avenue for carbon neutrality. The renewable-energy-powered electrochemical CO<sub>2</sub> reduction (eCO<sub>2</sub>R) process, particularly over Cu-based electrocatalysts, is a valuable asset for our decarbonization efforts to avoid climate consequences. Intending to enhance process efficiency, this work is a distinctive case study emphasizing the need to develop electrocatalysts in conjunction with adjusting operating conditions. A representative case is presented using fluorine-modified CuIn bimetallic electrocatalysts with tunable In/Cu ratios, demonstrating how to alter selectivity preferences based on reactor configuration: Our optimized catalyst system led to the highest faradaic efficiency (FE) for C<sub>2+</sub> products of 68 % and the highest C<sub>1</sub> FE of 80 % using gas diffusion electrodes (GDE)- and H-cell-type based electrolyzer, respectively. Moreover, the controllable In/Cu ratio and the degree of fluoride doping played a pivotal role in governing the physicochemical properties of the bimetallic electrocatalysts and their eCO<sub>2</sub>R performance. Diverse characterization tools offered systematic insights into the relationships between catalyst structure and properties, reactor configuration, electrolyte, and performance, aiming to enhance the Technology Readiness Level of the eCO<sub>2</sub>R process.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"439 ","pages":"Article 115768"},"PeriodicalIF":6.5,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142315600","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Synthesis of high surface area mesoporous ZnAl2O4 with excellent photocatalytic activity for the photodegradation of Congo Red dye 合成具有优异光催化活性的高比表面积介孔 ZnAl2O4，用于光降解刚果红染料

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-20 DOI: 10.1016/j.jcat.2024.115769

S.A.A. Shah , N. Gkoulemani , J.T.S. Irvine , M.T. Sajjad , R.T. Baker

{"title":"Synthesis of high surface area mesoporous ZnAl2O4 with excellent photocatalytic activity for the photodegradation of Congo Red dye","authors":"S.A.A. Shah , N. Gkoulemani , J.T.S. Irvine , M.T. Sajjad , R.T. Baker","doi":"10.1016/j.jcat.2024.115769","DOIUrl":"10.1016/j.jcat.2024.115769","url":null,"abstract":"<div><div>The large-scale release by the textile and other industries of organic dyes into water courses degrades the aquatic environment and results in serious health problems for wildlife, humans, and domestic animals. The removal of such dyes from wastewater is therefore a pressing and important challenge. The efficient photocatalytic destruction of these dyes using sunlight is an elegant and attractive potential solution. In this work, mesoporous ZnAl<sub>2</sub>O<sub>4</sub> nanomaterials were prepared with high specific surface area, high pore volume and uniform pore size distribution using a modified sol–gel synthetic protocol. BET analysis showed that the highest surface area achieved for ZnAl<sub>2</sub>O<sub>4</sub> reached 344 m<sup>2</sup>/g. The texture, structure and chemical composition of these materials were further studied using XRD, FTIR, TEM, EDS, CHN and XPS analysis and zeta potential measurements. Band gap energies were obtained from UV/vis spectra and showed a strong decrease as particle size decreased, shifting absorption into the visible range for the finest materials and indicating the potential to improve the efficiency of photocatalysis under solar irradiation. Photocatalytic activity was evaluated by studying the photodegradation of Congo Red dye and, for the best materials, showed that 99 % of the dye was degraded in only 30 mins. These results compared very favourably with those of previously reported studies. The degradation products of the Congo Red were further investigated using mass spectrometry and this detailed study confirmed that true photoinduced fragmentation of the dye molecule occurred rather than simple ‘photobleaching’.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"439 ","pages":"Article 115769"},"PeriodicalIF":6.5,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142319230","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Enhancing CO tolerance in hydrogen oxidation reaction through synergy of surface-modified MoOx with PtRu alloy 通过表面改性氧化钼与铂钌合金的协同作用，提高氢氧化反应中的一氧化碳耐受性

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-20 DOI: 10.1016/j.jcat.2024.115767

Yan-Qi Jin , Qi Wang , Si-Yi Tian , Hong-Bin Zeng , Jun-Fei Shen , Zhi-Ming Zhang , Tao Wang , Na Tian , Zhi-You Zhou , Shi-Gang Sun

{"title":"Enhancing CO tolerance in hydrogen oxidation reaction through synergy of surface-modified MoOx with PtRu alloy","authors":"Yan-Qi Jin , Qi Wang , Si-Yi Tian , Hong-Bin Zeng , Jun-Fei Shen , Zhi-Ming Zhang , Tao Wang , Na Tian , Zhi-You Zhou , Shi-Gang Sun","doi":"10.1016/j.jcat.2024.115767","DOIUrl":"10.1016/j.jcat.2024.115767","url":null,"abstract":"<div><div>Even trace amounts of CO impurities present in low-cost crude hydrogen can severely poison Pt-based catalysts. For proton exchange membrane fuel cells (PEMFCs), the development of hydrogen oxidation reaction (HOR) catalysts capable of enduring CO contamination is of significant economic importance. In this study, we propose a new strategy to synergistically enhance the CO tolerance of PtRu alloys by incorporating MoO<sub>x</sub>. The MoO<sub>x</sub> modified on PtRu/C catalysts can initiate the oxidation of CO adsorbed on its surface at potentials as low as 0.125 V. The synergy effect of MoO<sub>x</sub> and bifunctional PtRu ensures sufficient HOR stability even under hydrogen containing high CO concentrations. The resulting PtRu-MoO<sub>x</sub>/C catalyst exhibits a 4.6-fold increase in the remained HOR current compared with commercial PtRu/C, after two hours in a hydrogen environment containing 10,000 ppm CO. Under typical testing condition of H<sub>2</sub>/1,000 ppm CO, PtRu-MoO<sub>x</sub>/C maintains over 80% of the initial current density even after ten hours, significantly outperforming PtRu/C (30%) and most previously reported catalysts.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"439 ","pages":"Article 115767"},"PeriodicalIF":6.5,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142311457","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Machine learning-based design of pincer catalysts for polymerization reaction 基于机器学习的聚合反应钳形催化剂设计

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-19 DOI: 10.1016/j.jcat.2024.115766

Shrabani Dinda , Tanvi Bhola , Suyash Pant , Anand Chandrasekaran , Alex K. Chew , Mathew D. Halls , Madhavi Sastry

{"title":"Machine learning-based design of pincer catalysts for polymerization reaction","authors":"Shrabani Dinda , Tanvi Bhola , Suyash Pant , Anand Chandrasekaran , Alex K. Chew , Mathew D. Halls , Madhavi Sastry","doi":"10.1016/j.jcat.2024.115766","DOIUrl":"10.1016/j.jcat.2024.115766","url":null,"abstract":"<div><div>We present a generic machine learning (ML) workflow for rapid screening of 3d-transition metal pincer catalysts utilizing bis(imino)pyridine ligands for homogeneous polymerization reactions. In this study, we compiled a dataset comprising over 503 catalysts. We identified the best quantitative structure–activity relationship (QSAR) models among hundreds, including both categorical and continuous, to predict catalytic activity, combining molecular fingerprints and descriptors. Top-performing models achieve high accuracy with coefficient of determination (R<sup>2</sup>) of nearly 80% for test sets; further validated by 5-fold cross-validation. We devised a mechanism to filter the outliers, such as ligands with <em>meta</em>-substituted groups. Steric map and QM-based descriptors like NBO charge, spin, HOMO-LUMO gap, and Fukui indices are identified as important features. <em>In silico</em> catalysts were generated by enumeration at <em>ortho</em> positions with bulky ligands like CHPh<sub>2</sub>, CH(p-F-Ph)<sub>2</sub>; directly linked with buried volume. This work supports increased innovation and accelerated development of new pincer catalysts using ML-based predictive modeling.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"439 ","pages":"Article 115766"},"PeriodicalIF":6.5,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324105","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Nickel-Catalyzed Cyclization/Thiocarbonylation of Alkene-Tethered indoles with sulfonyl Chlorides: Synthesis of Thioester-Substituted Indolo[2,1-a]isoquinolines 镍催化烯系吲哚与磺酰氯的环化/硫代羰基化反应：硫酯取代的吲哚并[2,1-a]异喹啉的合成

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-18 DOI: 10.1016/j.jcat.2024.115765

Chen-Yang Hou , Hucheng Ma , Ruyi Zhao , Xinxin Qi , Xiao-Feng Wu

引用次数: 0

Nickel-catalyzed thiocarbonylation for the synthesis of thioesters-functionalized 2H-pyrones with sulfonyl chlorides as the sulfur sources 镍催化的硫代羰基化反应，以磺酰氯为硫源合成硫代酯官能化的 2H-pyrones

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-18 DOI: 10.1016/j.jcat.2024.115764

Chen-Yang Hou , Hucheng Ma , Ruyi Zhao , Xinxin Qi , Xiao-Feng Wu

引用次数: 0

Atomically dispersed Zn sites on N-doped carbon boosted transesterification of symmetrical organic carbonates with biomass-derived alcohols 掺杂 N 的碳上原子分散的 Zn 位点促进了对称有机碳酸盐与生物质衍生醇的酯交换反应

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-17 DOI: 10.1016/j.jcat.2024.115763

Yayun Pang , Long Tao , Ziyang Wang , Chenglei Xiao , Kaili Wang , Kongqian Liang , Jinliang Song , Tiejun Wang

{"title":"Atomically dispersed Zn sites on N-doped carbon boosted transesterification of symmetrical organic carbonates with biomass-derived alcohols","authors":"Yayun Pang , Long Tao , Ziyang Wang , Chenglei Xiao , Kaili Wang , Kongqian Liang , Jinliang Song , Tiejun Wang","doi":"10.1016/j.jcat.2024.115763","DOIUrl":"10.1016/j.jcat.2024.115763","url":null,"abstract":"<div><p>Transesterification of symmetrical organic carbonates with alcohols to access the unsymmetrical ones is a highly attractive strategy for upgrading biomass-derived alcohols. Robust, facile-prepared, and cost-effective catalytic materials remain highly desirable for this route. Herein, we designed several Zn-based catalysts (denoted as Zn@C-T, where T represented the pyrolysis temperature) by the pyrolysis of Zn-based coordination polymer at different temperatures. Very interestingly, the prepared Zn@C-900 could efficiently catalyze the transesterification of diethyl carbonate (DEC) with various biomass-derived alcohols to synthesize the corresponding unsymmetrical organic carbonates with high yields (>95 %), resulting from the atomically dispersed ZnN<sub>x</sub> sites on the N-doped carbon. Notably, good catalytic activity could be obtained at a low temperature of 80 °C, representing the major breakthrough. Detailed investigations indicated that the excellent performance of Zn@C-900 originated mainly from the synergistic effect of Zn (to activate DEC) and N (to activate the alcohols) in the ZnN<sub>x</sub> sites. This work provided a promising efficient catalyst for low-temperature production of unsymmetrical organic carbonates <em>via</em> transesterification of DEC.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"439 ","pages":"Article 115763"},"PeriodicalIF":6.5,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142244237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Facilitating photocatalytic CO2 methanation via synergetic feed of photon-induced carriers and reactants over S-scheme BiVO4@TiO2 nanograss/needle arrays 通过 S 型 BiVO4@TiO2 纳米草/针阵列上光子诱导载流子和反应物的协同供给促进光催化二氧化碳甲烷化

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-16 DOI: 10.1016/j.jcat.2024.115760

Dawei Zhao, Yimin Xuan, Chen Sun, Longzhen Zhang, Qibin Zhu, Xianglei Liu

{"title":"Facilitating photocatalytic CO2 methanation via synergetic feed of photon-induced carriers and reactants over S-scheme BiVO4@TiO2 nanograss/needle arrays","authors":"Dawei Zhao, Yimin Xuan, Chen Sun, Longzhen Zhang, Qibin Zhu, Xianglei Liu","doi":"10.1016/j.jcat.2024.115760","DOIUrl":"10.1016/j.jcat.2024.115760","url":null,"abstract":"<div><p>Herein, a unique structure BiVO<sub>4</sub>@TiO<sub>2</sub> nanograss/needle arrays S-scheme heterojunction photocatalyst for CO<sub>2</sub> photoreduction reaction was created. The photocatalyst can drive electrons to the reactive spots spontaneously and continuously, which effectively tackles the problem of severe recombination and disordered migration of photogenerated carriers. Theoretical calculations and experimental results demonstrate that adding BMIM-BF<sub>4</sub> ionic liquid to generate BMIM-*CO<sub>2</sub> intermediate promotes CO<sub>2</sub> activation and enrichment of reactants concentration around the catalytic sites. Benefiting from the sufficient electron supply of catalytic sites and reinforced reactants supply in the interfacial microenvironment, the BiVO<sub>4</sub>@TiO<sub>2</sub> photocatalyst shows high selectivity and activity of CO<sub>2</sub>-to-CH<sub>4</sub> conversion. The CH<sub>4</sub> selectivity increased to 57.3 % (132.7 μmol m<sup>-2</sup>h<sup>−1</sup>) and the methanation activity was increased by 8.6 times in the 5.0 % BMIM-BF<sub>4</sub> aqueous solution. Significantly, the BiVO<sub>4</sub>@TiO<sub>2</sub> NNAs catalyst obtains a solar-to-fuels energy efficiency of ∼ 0.46 ‰ under ultraviolet-enhanced light sources without any sacrificial agent or co-catalyst. This work displays the relationship between reaction process factors (electron supply, CO<sub>2</sub> molecule, and proton supply) and CO<sub>2</sub> photoreduction activity and selectivity, giving new insight into achieving efficient CO<sub>2</sub> photoreduction conversion.</p></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"439 ","pages":"Article 115760"},"PeriodicalIF":6.5,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142244235","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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Chiral metal complexes: Design strategies for precision in asymmetric C–H activation 手性金属配合物：实现不对称 C-H 激活精确性的设计策略

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2024-09-16 DOI: 10.1016/j.jcat.2024.115756

Devesh Chandra , Tammana Sharma , Sarthi , Sachin , Upendra Sharma

引用次数: 0