Journal of Catalysis最新文献

{"title":"Electron-withdrawing effect of polyoxometalates in Cu(I)-based metal–organic frameworks for enhanced azide-alkyne “click” reaction","authors":"Bing-Bing Lu ,&nbsp;Ji-Qiang Guan ,&nbsp;Yu-Tong Wu ,&nbsp;Si-Yi An ,&nbsp;Ying Fu ,&nbsp;Fei Ye","doi":"10.1016/j.jcat.2024.115818","DOIUrl":"10.1016/j.jcat.2024.115818","url":null,"abstract":"<div><div>Boosting the nucleophilicity of Cu(I) sites is an essential strategy to enhance the efficiency of Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) reaction. In this work, a Lindquist-type polyoxometalate (POM)-based metal–organic framework, [Cu^I₄(W₆O₁₉)₂(L)]·2H₂O (NEAU-1), was synthesized via an in-situ solvothermal method. Single-crystal X-ray diffraction results reveal that NEAU-1 exhibits a sandwich structure, with POMs intercalated between the two-dimensional layers formed by resorcin[4]arene ligands and Cu(I) ions. NEAU-1 possesses abundant Cu(I) active sites and high chemical stability, making it an effective heterogeneous catalyst for the CuAAC reaction. More importantly, the presence of POMs effectively reduces the electron cloud density around Cu(I) sites, significantly lowering the energy barrier for the formation of copper-acetylide compounds and facilitating subsequent nucleophilic reactions. The synergistic catalytic effect of POMs and Cu(I) can achieve a conversion rate of over 99 % for benzyl azide and phenylacetylene within 40 min. This work presents a sustainable molecular-level strategy to enhance the activity of the CuAAC reaction.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115818"},"PeriodicalIF":6.5,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142486829","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}

{"title":"Highly stable and electron-rich Ni single atom catalyst for directed electroreduction of CO2 to CO","authors":"Fengwei Zhang ,&nbsp;Jijie Li ,&nbsp;Shuai Chen ,&nbsp;Jingjing Li ,&nbsp;Ruimin Zhang ,&nbsp;Yangyang Zhao ,&nbsp;Wen-Yan Zan ,&nbsp;Yawei Li","doi":"10.1016/j.jcat.2024.115815","DOIUrl":"10.1016/j.jcat.2024.115815","url":null,"abstract":"<div><div>Transition metal-nitrogen-carbon (M−N−C) are considered as promising candidates for the electrochemical conversion of inert CO₂ into high value-added CO products. However, previous reports have focused on Ni single-atom sites (Ni SAs) and the role of Ni nanoparticles (Ni NPs) in CO₂ electroreduction reaction (CO₂RR) has been overlooked. Herein, we prepared a series of Ni, N-codoped porous carbon (NiNC-T, T represents the temperature) catalysts by combining Ni phthalocyanine pyrolysis and acid etching strategy, which either contain only Ni SAs or both Ni SAs and Ni NPs. Notably, the NiNC-1100 catalyst with both Ni SAs and Ni NPs exhibited 99 % CO faradaic efficiency (FE_CO) at −0.66 V versus reversible hydrogen electrode (<em>vs.</em> RHE) and FE_CO above 98 % over a wide potential range (−0.66 V ∼  −1.06 V). Moreover, the FE_CO of NiNC-1100 remained above 95 % after 100 h of continuous electrocatalysis, which was significantly superior to that of the most advanced Ni single atom electrocatalysts. The systematic characterization results showed that the introduction of Ni NPs can promote the adsorption and activation of CO₂ by increasing the electron cloud density of Ni SAs, thus enhancing the CO₂RR catalytic performance.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115815"},"PeriodicalIF":6.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452585","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}

{"title":"Anion intercalation of NiMn-LDH accelerating urea electrooxidation on trivalent nickel","authors":"Qian Zheng ,&nbsp;Yuandong Yan ,&nbsp;Shaonan Zhang ,&nbsp;Shicheng Yan ,&nbsp;Zhigang Zou","doi":"10.1016/j.jcat.2024.115814","DOIUrl":"10.1016/j.jcat.2024.115814","url":null,"abstract":"<div><div>Reducing the urea oxidation reaction (UOR) barriers is a key knot for accelerating its practical applications. Here, we demonstrate that NiMn-LDH with sulfate anion interaction can enable urea electrooxidation with a low anodic potential of 1.36 V at 100 mA cm⁻². We find that the UOR on NiMn-LDH is driven by Ni³⁺ species and the Ni³⁺ generation is the rate-determining step of UOR. Both the Mn doping and sulfate anion interaction contribute to the low-barrier phase transformation from Ni(OH)₂ to NiOOH to produce the Ni³⁺ state with high activity in UOR, owing to that Mn doping optimizes the electronic states and intercalation of guest anions weakens the interlayer interactions, which ultimately tunes Ni³⁺ generation kinetics toward the superior UOR activity. Our findings provide new insights into the design of the highly active UOR catalysts.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115814"},"PeriodicalIF":6.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452587","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}

{"title":"Stability of supported Pd-based ethanol oxidation reaction electrocatalysts in alkaline media","authors":"Tuani C. Gentil ,&nbsp;Maria Minichova ,&nbsp;Valentín Briega-Martos ,&nbsp;Victor S. Pinheiro ,&nbsp;Felipe M. Souza ,&nbsp;João Paulo C. Moura ,&nbsp;Júlio César M. Silva ,&nbsp;Bruno L. Batista ,&nbsp;Mauro C. Santos ,&nbsp;Serhiy Cherevko","doi":"10.1016/j.jcat.2024.115816","DOIUrl":"10.1016/j.jcat.2024.115816","url":null,"abstract":"<div><div>This study evaluates the dissolution of the supported electrocatalysts Pd/C, PdSn/C, PdNb/C, and PdFe₃O₄/C during ethanol oxidation reaction for Alkaline Direct Liquid Fuel Cells (ADLFC) applications. A scanning flow cell (SFC) combined to an inductively coupled plasma mass spectrometry (online ICP-MS) is used to assess the dissolution stability in a broad potential window. Accelerated stress tests with and without ethanol are developed using a rotating disk electrode (RDE) with dissolution products analysis by ex-situ ICP-MS. Potential profiles simulating those experienced by the catalyst during regular fuel cell operation were used. Sn and Fe catalysts demonstrate improved activity and stability compared with the material with Pd alone. For these reasons, PdSn/C and PdFe₃O₄/C are suitable for ADLFC applications. Severe Nb dissolution destabilizes Pd, increasing its leaching. This work demonstrates that while additional metals and oxides can improve the alcohol oxidation kinetics of Pd, these additives’ dissolution stability must already be considered at the catalyst design stage.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115816"},"PeriodicalIF":6.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452586","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}

{"title":"Plasmon and N-vacancy synergistically enhanced tubular carbon nitride-based S-scheme heterojunction photocatalyst with one stone five birds function: Pathways, DFT calculation and mechanism insight","authors":"Feng Sun,&nbsp;Qian Xu,&nbsp;Haiyang Liu,&nbsp;Da Xu,&nbsp;Xinxing Wang,&nbsp;Chuan Luo,&nbsp;Tianqi Wang,&nbsp;Hui Yu,&nbsp;Wensheng Yu,&nbsp;Xiangting Dong","doi":"10.1016/j.jcat.2024.115813","DOIUrl":"10.1016/j.jcat.2024.115813","url":null,"abstract":"<div><div>From the perspectives of innovation and broad-spectrum, tubular carbon nitride-based photocatalyst, <em>viz.</em>, Ag/AgI/g-C₃N₄ S-scheme heterojunction photocatalyst, with enhancement of nitrogen vacancy and localized surface plasmon resonance (LSPR) effect is reasonably devised and manufactured <em>via</em> combining hydrothermal, calcination and photo-reduction techniques. The optimal specimen displays high photocatalytic activity in removal of dyes [such as crystal violet (CV), 100.00 %/60 min], antibiotics [such as levofloxacin (LEV), 88.72 %/50 min] and Cr(VI) (100.00 %, 30 min), photocatalytic hydrogen evolution (1023.3 μmol h⁻¹ g⁻¹) and H₂O₂ generation (866.2 μmol h⁻¹ g⁻¹), achieving broad-spectrum natures, <em>viz.</em>, realizing the function of “one stone five birds”. The broad-spectrum natures are attributed to the synergisms of nitrogen vacancy, LSPR effect of Ag, hollow tube structure and S-scheme heterojunction, which facilitate the separation and migration of photo-generated carriers and inject “hot electrons” generated by Ag into the conduction band of Ag/AgI/g-C₃N₄, increase the specific surface area and broaden the spectral response range. Further, the degraded intermediates of CV and LEV and possible degradation pathways are rationally advanced by the aid of LCMS spectra, the predicted toxicity of degraded intermediates of LEV is assessed by Toxicity Estimation Software (T.E.S.T.), and the biotoxicity of CV, LEV and Cr(VI) solutions after photocatalytic degradation is further assessed by feat of cultivate rice. Synergistically enhanced photocatalytic mechanism of Ag/AgI/g-C₃N₄ hollow tube S-scheme heterojunction is confirmed based upon a series of sound experiments, fs-TA spectra, in-situ XPS and DFT calculation, <em>etc</em>.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115813"},"PeriodicalIF":6.5,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452588","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}

{"title":"1,6-Conjugate hydrogenation of para-quinone methides to phenol-containing diaryl- and triarylmethanes under atmospheric pressure catalyzed by a metal–ligand bifunctional iridium catalyst","authors":"Guoqiang Zhao ,&nbsp;Xiangchao Xu ,&nbsp;Jin Zhang ,&nbsp;Beixuan Dong ,&nbsp;Wenli Wang ,&nbsp;Wenbo Zhou ,&nbsp;Qixun Shi ,&nbsp;Feng Li","doi":"10.1016/j.jcat.2024.115812","DOIUrl":"10.1016/j.jcat.2024.115812","url":null,"abstract":"<div><div>The 1,6-conjugate hydrogenation of <em>para</em>-quinone methides to diaryl- and triarylmethanes under atmospheric pressure has been proposed and accomplished. In the presence of [Cp*Ir(2,2′-bpyO)(H₂O)] (0.5 mol %), a range of desirable products were obtained in high yields. Functional groups in bpy ligand were found to be crucially important for the catalytic activity of iridium complexes. Furthermore, the practical application of the present catalytic system was also presented.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115812"},"PeriodicalIF":6.5,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142451616","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}

{"title":"Abundant interfacial and intrinsic oxygen vacancies enabling small nickel/ceria nanocrystal efficient CO2 methanation","authors":"Chaoyang Yang,&nbsp;Junlei Zhang,&nbsp;Weiping Liu,&nbsp;Xueyi Yang,&nbsp;Yuwen Wang,&nbsp;Wanglei Wang","doi":"10.1016/j.jcat.2024.115811","DOIUrl":"10.1016/j.jcat.2024.115811","url":null,"abstract":"<div><div>Smaller nano-sizes typically result in supported catalysts with abundant interfacial and intrinsic oxygen vacancies for better adsorption and activation of small molecules, including CO₂, leading to improved efficiency of CO₂ methanation. Here, Ni/CeO₂-S with the smaller nano-size of around 4.2 nm is used to catalyze CO₂ methanation, which exhibits significantly enhanced activity compared to larger nano-sized Ni/CeO₂-L catalyst, even surpassing the most majority of previously reported catalysts using CeO₂ as the support or Ni as the active metal. The coexistence of interfacial defects and intrinsic oxygen vacancies allows for enhanced adsorption and activation of CO₂ molecules as well as H spillover, resulting in such improved CO₂ methanation. <em>In-situ</em> DRIFTS demonstrate a nearly sole Formate pathway on Ni/CeO₂-S for efficient CO₂ hydrogenation. This research provides valuable insights into the reaction mechanism over a small nanosize supported catalyst.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115811"},"PeriodicalIF":6.5,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142450150","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}

{"title":"Water-assisted preparation of Ni/La(OH)3 catalyst for efficient catalytic C-O bond hydrogenolysis of tetrahydrofuran-dimethanol","authors":"Xinyu Yao ,&nbsp;Dong Liu ,&nbsp;Junhong Fu ,&nbsp;Jian Wang ,&nbsp;Mengle Shen ,&nbsp;Zuoyi Xiao ,&nbsp;Qingda An ,&nbsp;Jiahui Huang","doi":"10.1016/j.jcat.2024.115790","DOIUrl":"10.1016/j.jcat.2024.115790","url":null,"abstract":"<div><div>Due to easy dehydration of La(OH)₃ to LaOOH by thermal treatment, it is challenging to prepare highly efficient Ni/La(OH)₃ catalyst for hydrogenolysis reactions. Herein, Ni/La(OH)₃ (Ni/La-2) catalyst is prepared by thermal reduction of NiO/La(OH)₃ in hydrogen flow with vaporized water, while La(OH)₃ is partially dehydrated to LaOOH without water vapor affording Ni/(La(OH)₃ + LaOOH) (Ni/La-1). Ni/La-2 displays 93 % and 3 % yields of 1,2,6-hexanetriol (HTO) and 1,6-hexanediol (HDO) respectively towards C-O hydrogenolysis of tetrahydrofuran-dimethanol (THFDM) in batch reactor and high stability (200 h) in fixed-bed reactor, which is the best among the reported catalysts to the best of our knowledge. Ni/La-2 possesses pure La(OH)₃ as support, enhanced dispersion of Ni species and abundant Ni^δ+-O-La interfaces in comparison to Ni/La-1, which results in the exceptional catalytic performances in C-O hydrogenolysis of THFDM. A fine control of reaction temperature and time is required to optimize the yields HTO and HDO in hydrogenolysis of THFDM over Ni/La-2. The water-assisted preparation method provides a new perspective for the preparation of La(OH)₃ supported metal catalysts.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115790"},"PeriodicalIF":6.5,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142450207","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}

{"title":"Bimodal mesoporous AlMCM-41 supported NiMo catalysts for efficient hydrodesulfurization of 4,6-dimethyldibenzothiophene","authors":"Hao Zhang,&nbsp;Qing Zhang,&nbsp;Guang-Ren Qian,&nbsp;Hong Liu,&nbsp;Yang Yue","doi":"10.1016/j.jcat.2024.115799","DOIUrl":"10.1016/j.jcat.2024.115799","url":null,"abstract":"<div><div>In this research, a bimodal mesoporous AlMCM-41 (B-AM41) material was prepared and applied to support NiMo catalysts for the hydrodesulfurization (HDS) of 4,6-dimethyldibenzothiophene. Additionally, catalysts supported on smaller and larger single-pore AlMCM-41 (S-AM41 and L-AM41) were also prepared as reference catalysts. Detailed characterizations show that the proportion, stacking degree, and length of the MoS₂ active phase on the different catalysts are distinct. As a result, HDS evaluation indicates that the NiMo/B-AM41 catalyst exhibited better catalytic activity with a reaction rate constant of 10.4 × 10⁻⁸ mol g⁻¹ s⁻¹ and a turnover frequency of 7.0 × 10⁻⁴ s⁻¹, significantly surpassing the S-AM41 and L-AM41 supported catalysts. The superior activity of the NiMo/B-AM41 catalyst can be attributed to a high sulfidation degree that provides sufficient highly dispersed type Ⅱ MoS₂ phases with minimal stacking and moderate slab length. Moreover, the bimodal mesoporous structure promotes the diffusion of 4,6-DMDBT and benefits its contact with active sites.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115799"},"PeriodicalIF":6.5,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142450149","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}

{"title":"Plasma-driven non-oxidative coupling of methane to ethylene and hydrogen at mild temperature over CuxO/CeO2 catalyst","authors":"Rui Liu ,&nbsp;Shangkun Li ,&nbsp;Qian Chen ,&nbsp;Dongxing Li ,&nbsp;Jiasong Zhao ,&nbsp;Chuang Li ,&nbsp;Xiaoxia Gao ,&nbsp;Wenping Zhao ,&nbsp;Li Wang ,&nbsp;Chong Peng ,&nbsp;Annemie Bogaerts ,&nbsp;Hongchen Guo ,&nbsp;Yanhui Yi","doi":"10.1016/j.jcat.2024.115810","DOIUrl":"10.1016/j.jcat.2024.115810","url":null,"abstract":"<div><div>We report one-step non-oxidative coupling of methane (CH₄) to ethylene (C₂H₄) at atmospheric pressure and mild temperature (ca. 180–190 °C), by a combination of non-thermal plasma and a CuO_x/CeO₂ catalyst. The C₂H₄ selectivity gradually increases during an induction period. The corresponding spent catalysts at different stages were systematically characterized to disclose the evolution of the CuO_x/CeO₂ catalyst. During the induction period, the CuO/CeO₂ catalyst was partially reduced to generate Cu⁺, Ce³⁺ and O_v species, which accompany the formation of Cu⁺-O_v-Ce³⁺ sites, as proven by XRD, HRTEM, XPS, Raman, EPR and H₂-TPR. In addition, the C₂H₄ selectivity is proportional to the fraction of Cu⁺, Ce³⁺, O_v and Cu-O-Ce species, which indicates that Cu⁺-O_v-Ce³⁺ is the active site for non-oxidative coupling of CH₄ to C₂H₄. Furthermore, <em>in-situ</em> FTIR results indicate that the Cu⁺-O_v-Ce³⁺ interface sites can promote dehydrogenation of CH₃* (from CH₄ plasma) to produce CH₂* on the catalyst surface, which is the basic reason why CuO_x/CeO₂ acts as a catalyst in speeding up the non-oxidative coupling of CH₄ for C₂H₄ production.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"440 ","pages":"Article 115810"},"PeriodicalIF":6.5,"publicationDate":"2024-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142450208","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}