Journal of Catalysis最新文献_第5页

Volcano-type relationship between oxidation states and H2O2 yield of Pd/TiO2 catalysts for direct synthesis of H2O2

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-12 DOI: 10.1016/j.jcat.2025.116069

Jiamei Wei , Xuning Wang , Shen Wang, Lin Zhu, Haoxiang Xu, Daojian Cheng

{"title":"Volcano-type relationship between oxidation states and H2O2 yield of Pd/TiO2 catalysts for direct synthesis of H2O2","authors":"Jiamei Wei , Xuning Wang , Shen Wang, Lin Zhu, Haoxiang Xu, Daojian Cheng","doi":"10.1016/j.jcat.2025.116069","DOIUrl":"10.1016/j.jcat.2025.116069","url":null,"abstract":"<div><div>The oxidation state of Pd species has been regarded as significant property to adjust catalytic performance for the direct synthesis of H2O2 (DSHP). However, the effect of oxidation state on DSHP remains controversial in whether higher or lower oxidation states benefit the enhancement of H2O2 yield. Herein, we discover a volcanic relationship between Pd oxidation state of Pd/TiO2 catalysts and H2O2 yield. A series of Pd/TiO2 catalysts were synthesized with controllable oxidation state via modifying heat treatment condition. Specifically, the Pd2+% has a volcanic relationship with H2O2 selectivity, while has an inverted volcanic relationship with H2 conversion, emerging with a summit of H2O2 yield at the moderate experimental oxidation state of Pd (Pd2+%=34.55%). Mechanism studies illustrate that the layered Pd oxides on metallic Pd have different oxidation degrees upon diverse heat treatment condition, which accounts for the Pd oxidation state dependent H2O2 yield on Pd/TiO2. The partial oxidation of metal Pd is regarded as the active site of the moderate oxidation state, which effectively hinder the hydrogenation and decomposition of H2O2 and first-order reaction to produce H2O. In this work, we emphasized the important role of oxidation state in regulating catalytic activity and selectivity, which provides guidance for the rational design of Pd-based catalysts towards DSHP.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116069"},"PeriodicalIF":6.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608450","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

Visible-light-induced C2-selective trifluoromethylation of indoles catalyzed by copper-containing covalent organic frameworks

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-11 DOI: 10.1016/j.jcat.2025.116077

Zhicheng Chen, Mengqi Zou, Xianghui Zhu, Huixin Tong, Zhizhong Sun, Wenyi Chu

引用次数: 0

Regulating the N-coordination environment of single-atom active sites in covalent organic frameworks for boosting photocatalytic CO2 reduction

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.jcat.2025.116078

Jing Wang , Jing Ning , Qingqing Tang , Lina Che , Ying-Ying Gu , Xusheng Wang , Xuefeng Wang , Long Hao , Li Shi

{"title":"Regulating the N-coordination environment of single-atom active sites in covalent organic frameworks for boosting photocatalytic CO2 reduction","authors":"Jing Wang , Jing Ning , Qingqing Tang , Lina Che , Ying-Ying Gu , Xusheng Wang , Xuefeng Wang , Long Hao , Li Shi","doi":"10.1016/j.jcat.2025.116078","DOIUrl":"10.1016/j.jcat.2025.116078","url":null,"abstract":"<div><div>The catalytic properties of single-atom catalysts with N atoms coordinated metal sites are highly dependent on their coordination environment, but a clear and systematic study of CO2 reduction performances affected by the type of coordinated N atoms is still lacking. Herein, by using Co single-atom incorporated covalent organic frameworks (COF) catalyst as a well-defined platform, we demonstrate that changing one coordinated N atom from pyrazine N to pyridine N can successfully improve the activity and selectivity of photocatalytic CO2 reduction in the presence of triethanolamine as sacrificial agent. Both the experimental and theoretical results reveal that regulating the type of coordinated N atoms can modulate the electronic structure of single-atom Co sites in COF, resulting in enhanced CO2 adsorption ability, improved electron trapping capability and reduced formation energy barriers of *COOH intermediate for facilitating CO2 reduction and simultaneously suppressing H2 evolution. This work sheds light on the significance of coordination atoms regulation in single-atom catalysts for improving catalytic performances.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"446 ","pages":"Article 116078"},"PeriodicalIF":6.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143589876","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

Ti-MOF-derived titanium oxide-modified carbon nitride: A Z-scheme heterostructure for the selective photocatalytic cleavage of lignin CC bonds

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.jcat.2025.116076

Yixin Li , Jianhao Qiu , Jie Xu , Yong Tang , Dingliang Dai , Guanglu Xia , Biyao Fang , Jianfeng Yao

{"title":"Ti-MOF-derived titanium oxide-modified carbon nitride: A Z-scheme heterostructure for the selective photocatalytic cleavage of lignin CC bonds","authors":"Yixin Li , Jianhao Qiu , Jie Xu , Yong Tang , Dingliang Dai , Guanglu Xia , Biyao Fang , Jianfeng Yao","doi":"10.1016/j.jcat.2025.116076","DOIUrl":"10.1016/j.jcat.2025.116076","url":null,"abstract":"<div><div>The utilization of solar energy to break the Cα<img>Cβ bonds in lignin under mild conditions is highly important for lignin valorization. This work presents an MIL-125-derived titanium oxide (M-TiO2)-modified carbon nitride (g-C3N4) heterostructure for selective photocatalytic lignin Cα<img>Cβ bond cleavage at room temperature. The conversion of lignin model 2-phenoxy-1-phenylethanol (PP-ol) reached 90.8 % over M-TiO2/g-C3N4 composites, which is visibly higher than that of bare M-TiO2 (33.2 %) and g-C3N4 (57.3 %). Furthermore, the selectivity of Cα<img>Cβ bond breakage reached 96.8 %, and the yield of benzaldehyde was as high as 86.4 %. A mechanistic study innovatively demonstrated that lignin Cα<img>Cβ bond cleavages are achieved by the cooperative effect between holes and 1O2, where holes dominate PP-ol conversion, whereas 1O2 governs Cα<img>Cβ bond cleavages. M-TiO2 has relatively large surface areas and high porosities, and the Z-scheme heterojunctions retard charge carrier recombination and outfit strong redox abilities, which separately prompt O2 adsorption and evolution to generate 1O2, accounting for the high selectivity of Cα<img>Cβ bond breakages over M-TiO2/g-C3N4 composites. This study sheds new light on the potential of metal–organic framework-derived materials in photocatalysis and provides valuable insights into the photocatalytic cleavage of lignin Cα<img>Cβ bonds.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"446 ","pages":"Article 116076"},"PeriodicalIF":6.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143589879","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

Hydrothermal assisted enhancing crystallinity of COF towards effective photocatalytic oxidation of benzylamines

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-06 DOI: 10.1016/j.jcat.2025.116058

Jiashi Chen , Xingyu Chen , Xiyue Cao , Huijuan Ma , Xuanfeng Jiang , Zhengguang Sun , Yuan Zhan

{"title":"Hydrothermal assisted enhancing crystallinity of COF towards effective photocatalytic oxidation of benzylamines","authors":"Jiashi Chen , Xingyu Chen , Xiyue Cao , Huijuan Ma , Xuanfeng Jiang , Zhengguang Sun , Yuan Zhan","doi":"10.1016/j.jcat.2025.116058","DOIUrl":"10.1016/j.jcat.2025.116058","url":null,"abstract":"<div><div>Photocatalysis is an environmentally friendly strategy for synthesis of high-value chemicals. However, covalent organic frameworks (COFs), as organic semiconductors, typically exhibit limited electrical conductivity, which significantly affects the photocatalytic efficiency of COF. In this work, a simple hydrothermal treatment method was presented to enhance the conductivity of aza-COF prepared by acid-catalyzed imine condensation of BTA⋅4HCl and HKH⋅8H2O. The crystallinity and carbonization degree of the aza-COF were explored by adjusting the hydrothermal temperatures from 80 to 160 °C. Remarkably, the COF-3 prepared by 120 °C hydrothermal temperature displays the highest photocatalytic conversion rate of benzylamine of 97 % with the high selectivity of 99 % in 4 h, outperforming the pristine aza-COF by 40 %. From various test results analysis, COF-3 exhibits the strongest transient photocurrent response, smallest electrochemical impedance, narrowest bandgap energy, attributed to its enhanced crystallinity, which improves conductivity. Furthermore, the photocatalysis mechanism was elucidated through quenching experiments, which determined the reactive oxygen species.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"446 ","pages":"Article 116058"},"PeriodicalIF":6.5,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569948","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

Efficient conversion of fructose to 5-hydroxymethylfurfural by hydrophobic modified SAPO-34 molecular sieve

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-06 DOI: 10.1016/j.jcat.2025.116059

Aojie Sun , Yu Ying , Meng Wang , Lin Zhu , Yidi Wang , Quan Zhang , Lanpeng Li , Changhai Cao , Haoxiang Xu , Daojian Cheng

{"title":"Efficient conversion of fructose to 5-hydroxymethylfurfural by hydrophobic modified SAPO-34 molecular sieve","authors":"Aojie Sun , Yu Ying , Meng Wang , Lin Zhu , Yidi Wang , Quan Zhang , Lanpeng Li , Changhai Cao , Haoxiang Xu , Daojian Cheng","doi":"10.1016/j.jcat.2025.116059","DOIUrl":"10.1016/j.jcat.2025.116059","url":null,"abstract":"<div><div>To address the issue of the accumulation of water around Brønsted acid sites during the fructose dehydration towards 5-hydroxymethylfurfural (HMF), in this work, hydrophobic SAPO-34 is prepared by post-treatment silanization by grafting alkyl hydrophobic groups on its surface. The SAPO-34 catalyst modified with dodecyl trimethoxysilane exhibits a significantly enhanced yield of 5-hydroxymethylfurfural (HMF), reaching 95.05 %. It is determined that long-chain hydrophobic groups facilitate the forward reaction of fructose dehydration by creating a microenvironment favorable for water removal and fructose enrichment. Furthermore, it releases Brønsted acid sites from water molecules, and enhance fructose’s accessibility to Brønsted acid sites. Thus, the activity, selectivity and durability of SAPO-34 can be promoted simultaneously, due to the selective removal water rather than fructose. This work put insight into the role of alkyl chain length of hydrophobic groups in promoting fructose dehydration towards HMF, which may be guideline for other dehydration reactions restricted by water.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"446 ","pages":"Article 116059"},"PeriodicalIF":6.5,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569950","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

Boost photoelectrocatalytic selectivity of glycerol to dihydroxyacetone on BiVO4 via accelerating middle hydroxyl oxidation by co-catalysts

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-06 DOI: 10.1016/j.jcat.2025.116061

Peixin Yang , Qianyang Chang , Qi Zhang , Jian Yu , Xing Ji , Ying Zhang , Wenjing Yang , Peng Xiao , Yunhuai Zhang

{"title":"Boost photoelectrocatalytic selectivity of glycerol to dihydroxyacetone on BiVO4 via accelerating middle hydroxyl oxidation by co-catalysts","authors":"Peixin Yang , Qianyang Chang , Qi Zhang , Jian Yu , Xing Ji , Ying Zhang , Wenjing Yang , Peng Xiao , Yunhuai Zhang","doi":"10.1016/j.jcat.2025.116061","DOIUrl":"10.1016/j.jcat.2025.116061","url":null,"abstract":"<div><div>Enhancing the selective oxidation of glycerol into 1,3-dihydroxyacetone (DHA) on a photoanode is attractive but challenging due to the complex reaction pathway. At present, the 20 % selectivity of DHA products on a BiVO4 photoanode in neutral condition as well as its photocorrosion prove to be below expectations. In this work, we decorated binary co-catalysts MnOx/FeOOH on BiVO4 (denoted BVO/Mn/Fe) for the selective photoelectrocatalytic glycerol to DHA. The BVO/Mn/Fe photoanode exhibited a DHA selectivity of 52 % at 1.2 VRHE with an evolution rate of 193.3 mmol m-2h−1 in pH = 7.0, and maintained 97.2 % of the initial photocurrent after 12 h stability test. The role of MnOx and FeOOH in the selective oxidation of glycerol was investigated through comprehensive spectroscopic and computational methods. Fourier transform infrared spectroscopy showed that the middle hydroxyl group preferentially adsorbs onto MnOx surfaces, density function theory calculations verified the optimized rate-determining step and decreased energy barrier by MnOx. Meanwhile, FeOOH significantly increased the active surface states on BiVO4 and produced more hydroxyl radicals. The synergistic effect of MnOx and FeOOH promoted the middle hydroxyl oxidation of glycerol and conversion efficiency to DHA on BiVO4 under neutral condition.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"446 ","pages":"Article 116061"},"PeriodicalIF":6.5,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569949","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

Innovative upcycling of polyesters and polycarbonates via manganese-catalyzed hydrogenolysis

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-06 DOI: 10.1016/j.jcat.2025.116060

Guoren Zhou , Chongyan Ren , Xiaoshi Zhang , Bocheng Xu , Maofu Pang , Xiaoxiao Chu

引用次数: 0

Promotional role of boron on Ni/SiO2 catalysts for dibenzofuran hydrodeoxygenation

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-05 DOI: 10.1016/j.jcat.2025.116056

Ting-Sheng Chen , Di Liu , Yun-Jie Li , Xing-Bao Wang , Chang-Hai Liang , Zhen-Yi Du , Wen-Ying Li

{"title":"Promotional role of boron on Ni/SiO2 catalysts for dibenzofuran hydrodeoxygenation","authors":"Ting-Sheng Chen , Di Liu , Yun-Jie Li , Xing-Bao Wang , Chang-Hai Liang , Zhen-Yi Du , Wen-Ying Li","doi":"10.1016/j.jcat.2025.116056","DOIUrl":"10.1016/j.jcat.2025.116056","url":null,"abstract":"<div><div>Controlling the oxygen-free product selectivity in catalytic hydrodeoxygenation is essential for producing high quality fuels from coal- and biomass-derived crude liquids. A series of boron-doped Ni/SiO2 catalysts were prepared for the efficient hydrodeoxygenation of dibenzofuran as a model compound. Boron doping significantly promoted the transformation of 2-cyclohexylcyclohexanol, which was accumulated as the main oxygen-containing intermediate compound on the pristine Ni/SiO2 catalyst, to the target products bicyclohexane and its isomer cyclopentylmethylcyclohexane. Characterization results show that boron doping increases Ni dispersion, modifies the electronic properties of Ni sites and in situ generates Brønsted acid sites by H2 spillover to boron oxides. The reduced Ni particle size improves the rates of dibenzofuran hydrogenation and 2-cyclohexylcyclohexanol dehydration. Electron-deficient Ni and boron oxides as the Lewis acid sites enhance the adsorption of 2-cyclohexylcyclohexanol. Furthermore, the in situ generated Brønsted acid sites favor the dehydration of 2-cyclohexylcyclohexanol, which gives the Ni-5B/SiO2 catalyst a better deoxygenation activity than the mechanical mixture of equal amounts of 5B/SiO2 and Ni/SiO2, as well as the one with a smaller Ni particle size of 3.8 nm.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"446 ","pages":"Article 116056"},"PeriodicalIF":6.5,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560922","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

Hydroamination of terminal alkynes mediated by W(0) complex: A convenient tool for new enamines synthesis

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-03-05 DOI: 10.1016/j.jcat.2025.116057

Izabela Czeluśniak , Paulina Pąchalska , Joanna Trojan-Piegza , Mariusz Majchrzak , Miłosz Siczek , Teresa Szymańska-Buzar

引用次数: 0