Applied Catalysis A: General最新文献

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Regulation of oxygen reduction pathway on carbon nitride for enhanced H2O2 photosynthesis 氮化碳氧还原途径对H2O2光合作用增强的调控
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-29 DOI: 10.1016/j.apcata.2025.120311
Bo Sheng, Jiarui Li, Jing Zhang
{"title":"Regulation of oxygen reduction pathway on carbon nitride for enhanced H2O2 photosynthesis","authors":"Bo Sheng,&nbsp;Jiarui Li,&nbsp;Jing Zhang","doi":"10.1016/j.apcata.2025.120311","DOIUrl":"10.1016/j.apcata.2025.120311","url":null,"abstract":"<div><div>Photocatalytic oxygen reduction reaction (ORR) to produce H<sub>2</sub>O<sub>2</sub> on graphitic carbon nitride (CN) has been regarded as a green and sustainable route by using endless solar energy. However, this process is limited by side-reactions of single electron transfer process, thus decreasing the overall efficiency. Herein, we have proposed an effective method to optimize H<sub>2</sub>O<sub>2</sub> photosynthesis by modulation of oxygen reduction pathway. That is modification of CN by introducing cyano groups and N defect in the presence of NaBH<sub>4</sub>. The H<sub>2</sub>O<sub>2</sub> production rate was 570 μmol/g/h by the optimal photocatalyst of BCN, showing 11-fold enhanced efficiency. Mechanism analysis proved that the convert of the single electron oxygen reduction in pristine CN into two-electron pathway in B<sub>x</sub>CN occurred, which contributed to improved ORR efficiency and accelerated conversion of O<sub>2</sub><sup>•−</sup> on H<sub>2</sub>O<sub>2</sub> photosynthesis. This work revealed an effective method for optimizing H<sub>2</sub>O<sub>2</sub> photosynthesis by regulating oxygen reduction reaction pathway.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"701 ","pages":"Article 120311"},"PeriodicalIF":4.7,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143907951","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Sulfur-enhanced ethanol dehydrogenation on fully exposed molybdenum clusters catalyst 全暴露钼团簇催化剂上的硫增强乙醇脱氢
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-29 DOI: 10.1016/j.apcata.2025.120316
Lei Zhu , Qiao Yuan , Xiangen Song , Lihua Shi , Yue Zhang , Siquan Feng , Xingju Li , Yutong Cai , Wenhao Cui , Li Yan , Dan Meng , Yunjie Ding
{"title":"Sulfur-enhanced ethanol dehydrogenation on fully exposed molybdenum clusters catalyst","authors":"Lei Zhu ,&nbsp;Qiao Yuan ,&nbsp;Xiangen Song ,&nbsp;Lihua Shi ,&nbsp;Yue Zhang ,&nbsp;Siquan Feng ,&nbsp;Xingju Li ,&nbsp;Yutong Cai ,&nbsp;Wenhao Cui ,&nbsp;Li Yan ,&nbsp;Dan Meng ,&nbsp;Yunjie Ding","doi":"10.1016/j.apcata.2025.120316","DOIUrl":"10.1016/j.apcata.2025.120316","url":null,"abstract":"<div><div>Ethanol dehydrogenation is of great industrial significance, but remains a challenge to use non-oxidative pathways. In this paper, Mo sites in different states were carefully constructed on sulfur-doped carbon (S-C) by adjusting the thermal treatment conditions, which showed distinct performance in the direct heterogeneous dehydrogenation of ethanol to acetaldehyde and ethyl acetate. Among them, Mo<sub>n</sub>/S-C with fully exposed molybdenum clusters anchored by sulfur sites showed the best performance with a space-time yield (STY) of 550 g<sub>acetyl</sub>/kg<sub>cat.</sub>/h and a selectivity of 92 % for the target acetyl product, which can be stable for more than 70 h. The Mo<sup>6 +</sup> species with electronic property modulated by sulfur were the active sites for ethanol dehydrogenation. The coordination-dependent catalytic performance was rationalized through possible reaction pathways, which demonstrated the evolution of active species during the reaction.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"701 ","pages":"Article 120316"},"PeriodicalIF":4.7,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143891063","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
ZnO supported on zinc spinel structures enabling the direct conversion of CO2 to olefins when combined with acidic CHA catalysts ZnO负载在锌尖晶石结构上,当与酸性CHA催化剂结合时,可以将CO2直接转化为烯烃
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-28 DOI: 10.1016/j.apcata.2025.120313
M.T. Nikolajsen , N.C. Schjødt , U.V. Mentzel , J. Sehested , R.Y. Brogaard , J.M. Christensen , M. Høj
{"title":"ZnO supported on zinc spinel structures enabling the direct conversion of CO2 to olefins when combined with acidic CHA catalysts","authors":"M.T. Nikolajsen ,&nbsp;N.C. Schjødt ,&nbsp;U.V. Mentzel ,&nbsp;J. Sehested ,&nbsp;R.Y. Brogaard ,&nbsp;J.M. Christensen ,&nbsp;M. Høj","doi":"10.1016/j.apcata.2025.120313","DOIUrl":"10.1016/j.apcata.2025.120313","url":null,"abstract":"<div><div>Bi-functional oxide-zeotype catalytic systems can convert CO<sub>2</sub> to light olefins, but at low conversions. Knowledge of the active sites for methanol synthesis over the oxide and the synergy with the zeotype at different operating conditions can guide future improvements. Here we investigate catalysts based on H-SAPO-34 combined with either ZnAl<sub>2</sub>O<sub>4</sub> or ZnGa<sub>2</sub>O<sub>4.</sub> We show that the methanol synthesis activity of the metal oxide is dependent on the Zn-content; the activity increases dramatically when Zn content exceeds the stoichiometric level, Zn/(Zn + M) &gt; 0.33 for M = Al or Ga. This creates supported surface ZnO domains, which selectively produce methanol and DME. Combining either of the Zn-spinel catalysts with H-SAPO-34 showed a light olefin selectivity &gt; 70 carbon mol% among the hydrocarbon products, but at a low CO<sub>2</sub> to hydrocarbon conversion of ∼3 %. Co-feeding CO increased the CO<sub>2</sub> to hydrocarbon conversion significantly without affecting the olefin selectivity.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"701 ","pages":"Article 120313"},"PeriodicalIF":4.7,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143912728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Ionic liquid-assisted N-formylation of morpholine with carbon dioxide and hydrogen catalyzed by N,P-ruthenium knitted aromatic polymers N, p -钌编织芳香族聚合物催化离子液体辅助啉啉与二氧化碳和氢的N-甲酰化反应
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-28 DOI: 10.1016/j.apcata.2025.120317
Li Luo , Boyu Zhu , Xinrong Wang, Jiao Geng, Xingbang Hu
{"title":"Ionic liquid-assisted N-formylation of morpholine with carbon dioxide and hydrogen catalyzed by N,P-ruthenium knitted aromatic polymers","authors":"Li Luo ,&nbsp;Boyu Zhu ,&nbsp;Xinrong Wang,&nbsp;Jiao Geng,&nbsp;Xingbang Hu","doi":"10.1016/j.apcata.2025.120317","DOIUrl":"10.1016/j.apcata.2025.120317","url":null,"abstract":"<div><div>The N-formylation reaction of amines with CO<sub>2</sub> is a promising method to utilize CO<sub>2</sub> for the production of high value-added chemicals. Herein, we developed an efficient process for integrating CO<sub>2</sub> capture and morpholine formylation catalyzed by a N,P-ruthenium knitted aromatic polymers (KAPs-N/Ru/P) catalyst, producing the corresponding N-formylmorpholine in good yield and high selectivity under relatively mild reaction conditions. TON up to 4711 can be achieved for the formylation of morpholine with CO<sub>2</sub> and H<sub>2</sub>, which represents the highest one for the reported heterogeneous Ru-based catalysts to date. The morpholine and CO<sub>2</sub> could be activated in the presence of ionic liquids and N-donor ligand (BPY). Simultaneously, phosphine ligand (PPh<sub>3</sub>) also contributed to the activation of H<sub>2</sub> and CO<sub>2</sub> based on DFT calculation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"701 ","pages":"Article 120317"},"PeriodicalIF":4.7,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143899860","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 phyllosilicate derived metal–acid bifunctional Ni/SiO2 catalysts for selective reductive amination of alcohols 层状硅酸盐镍衍生金属酸双官能团Ni/SiO2催化剂用于醇的选择性还原胺化反应
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-26 DOI: 10.1016/j.apcata.2025.120310
Qiongjin Jiang, Shiyi Rao, Zhenyu Yang, Xiao Fu, Weikun Chen, Linmin Ye , Youzhu Yuan
{"title":"Nickel phyllosilicate derived metal–acid bifunctional Ni/SiO2 catalysts for selective reductive amination of alcohols","authors":"Qiongjin Jiang,&nbsp;Shiyi Rao,&nbsp;Zhenyu Yang,&nbsp;Xiao Fu,&nbsp;Weikun Chen,&nbsp;Linmin Ye ,&nbsp;Youzhu Yuan","doi":"10.1016/j.apcata.2025.120310","DOIUrl":"10.1016/j.apcata.2025.120310","url":null,"abstract":"<div><div>The reductive amination of alcohols offers a cost-effective and sustainable pathway for the synthesis of amines. However, achieving high selectivity for primary amines remains a challenge. Herein, we report a nickel phyllosilicate catalyst (Ni/SiO<sub>2</sub>-AE) synthesized via ammonia evaporation, which demonstrates superior catalytic performance with 53.2% alcohol conversion and 96.2% primary amine selectivity. This outperforms conventional Ni/SiO<sub>2</sub> catalysts prepared by impregnation (16.5% conversion, 98.6% selectivity) and deposition-precipitation (41.3% conversion, 94.5% selectivity). The Ni/SiO<sub>2</sub>-AE catalyst exhibits remarkable stability over five reaction cycles, demonstrating both durability and recyclability. Characterization studies reveal that the high catalytic performance stems from the synergy between highly dispersed Ni<sup>0</sup> nanoparticles and Lewis acid sites derived from unsaturated Ni(II) species, which facilitate alcohol adsorption and activation. Additionally, the robust skeletal structure of nickel phyllosilicate contributes to the recyclability of the Ni/SiO<sub>2</sub>-AE catalyst. The metal–acid bifunctional Ni/SiO<sub>2</sub>-AE catalyst also displays broad substrate applicability, effectively converting diverse alcohols into their corresponding primary amines.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"701 ","pages":"Article 120310"},"PeriodicalIF":4.7,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143887276","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Constructing PtLa@ZnBeta catalyst with single atomic Pt catalyzing propane dehydrogenation 构建PtLa@ZnBeta单原子Pt催化丙烷脱氢催化剂
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-24 DOI: 10.1016/j.apcata.2025.120309
Wenli Zhao, Rui Zhou, Hongjiang Li, Shenmin Li, Yingna Cui, Xinping Wang
{"title":"Constructing PtLa@ZnBeta catalyst with single atomic Pt catalyzing propane dehydrogenation","authors":"Wenli Zhao,&nbsp;Rui Zhou,&nbsp;Hongjiang Li,&nbsp;Shenmin Li,&nbsp;Yingna Cui,&nbsp;Xinping Wang","doi":"10.1016/j.apcata.2025.120309","DOIUrl":"10.1016/j.apcata.2025.120309","url":null,"abstract":"<div><div>Zn has been found to be the most effective metal that geometrically and electrically modifies Pt by forming intermetallic alloy with Pt, whereas it suffers from gradual losing during the reaction caused by volatilization. Herein, we propose a strategy introducing La<sup>3 +</sup> together with Pt<sup>2+</sup> into the zeolite channels by ion-exchange that allow the La<sup>3+</sup> anchoring onto zeolite framework Zn and acting as the successor of Zn by forming alloy with Pt whereby executing the task of isolating and stabilizing the Pt atoms when Zn lost during the PDH reaction. The 0.3Pt0.32La@3ZnBeta(L) catalyst prepared in this way displayed much superior catalytic performance in PDH reaction than that of anchoring Pt<sup>2+</sup> cations alone onto framework Zn. It is worthy to extend this strategy to other metals that is capable of forming intermetallic alloy with Pt but possesses high boiling point, to develop highly active, selective and catalytic stable PDH catalysts.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"701 ","pages":"Article 120309"},"PeriodicalIF":4.7,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143891102","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Effect of catalyst support on dihydroeugenol hydrodeoxygenation on low cost FeNi catalyst to produce renewable alkane fuel 低成本FeNi催化剂对双氢丁香酚加氢脱氧制备可再生烷烃燃料的影响
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-23 DOI: 10.1016/j.apcata.2025.120307
Zuzana Vajglová , Päivi Mäki-Arvela , Olha Yevdokimova , Mark Martinez-Klimov , Irina Simakova , Kari Eränen , Teija Tirri , Jessi E.S. van Hoeven , Anssi Peuronen , Matej Huš , Blaž Likozar , Mika Lastusaari , Johan Lindén , Dmitry E. Doronkin , Dmitry Yu. Murzin
{"title":"Effect of catalyst support on dihydroeugenol hydrodeoxygenation on low cost FeNi catalyst to produce renewable alkane fuel","authors":"Zuzana Vajglová ,&nbsp;Päivi Mäki-Arvela ,&nbsp;Olha Yevdokimova ,&nbsp;Mark Martinez-Klimov ,&nbsp;Irina Simakova ,&nbsp;Kari Eränen ,&nbsp;Teija Tirri ,&nbsp;Jessi E.S. van Hoeven ,&nbsp;Anssi Peuronen ,&nbsp;Matej Huš ,&nbsp;Blaž Likozar ,&nbsp;Mika Lastusaari ,&nbsp;Johan Lindén ,&nbsp;Dmitry E. Doronkin ,&nbsp;Dmitry Yu. Murzin","doi":"10.1016/j.apcata.2025.120307","DOIUrl":"10.1016/j.apcata.2025.120307","url":null,"abstract":"<div><div>Solventless hydrodeoxygenation of dihydroeugenol was investigated in a continuous reactor at 300 °C under 30 bar over different nickel-iron catalysts, prepared using a two-step impregnation method. The following catalysts were studied: mesoporous FeNi/Al<sub>2</sub>O<sub>3</sub>, FeNi/SiO<sub>2</sub> and FeNi/H-MCM-48 as well as microporous FeNi/H-Beta-300, FeNi/H-Beta-38, FeNi/H-Y-5.1, FeNi/H-MCM-48 and FeNi/USY-30. The catalysts were characterized by SEM coupled with energy dispersive X-ray analysis, Mössbauer and X-ray absorption spectroscopy, hydrogen TPR, X-ray diffraction, TEM, nitrogen physisorption and FTIR pyridine adsorption. DFT calculations were performed to elucidate the role of Fe and Ni. The results revealed that FeNi/Al<sub>2</sub>O<sub>3</sub> was the most active and stable in dihydroeugenol hydrodeoxygenation. Complete conversion of dihydroeugenol was obtained and the yield of the main product propylcyclohexane was varying in the range 84–88 %. FeNi/Al<sub>2</sub>O<sub>3</sub> catalyst exhibited 3.4 nm metal particles and contained FeNi alloy particles with the fcc metallic structure. No deactivation was observed for FeNi/ Al<sub>2</sub>O<sub>3</sub> during 5 hours time-on-stream due to the presence of Ni-rich particles with iron-enriched outer surface confirmed by EXAFS. Fe was shown to be responsible for deoxygenation, while Ni promotes hydrogenation. Catalyst deactivation was observed for all other catalysts except for FeNi/Al<sub>2</sub>O<sub>3</sub> with increasing time-on-stream under the same reaction conditions due to their higher Brønsted to Lewis acid site ratio and larger average metal particle size in comparison to FeNi/Al<sub>2</sub>O<sub>3</sub>.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"701 ","pages":"Article 120307"},"PeriodicalIF":4.7,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143887275","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Solvent-free synthesis of mesoporous MoO3-V2O5/Al2O3 catalyst for liquid phase selective oxidation of furfural to maleic anhydride 无溶剂合成介孔MoO3-V2O5/Al2O3催化剂的液相选择性氧化糠醛制马来酸酐
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-22 DOI: 10.1016/j.apcata.2025.120308
Kasanneni Tirumala Venkateswara Rao , Donald R. Inns , Jeremy N. Winter , Troy D. Manning , John B. Claridge , Alexandros P. Katsoulidis , Matthew J. Rosseinsky
{"title":"Solvent-free synthesis of mesoporous MoO3-V2O5/Al2O3 catalyst for liquid phase selective oxidation of furfural to maleic anhydride","authors":"Kasanneni Tirumala Venkateswara Rao ,&nbsp;Donald R. Inns ,&nbsp;Jeremy N. Winter ,&nbsp;Troy D. Manning ,&nbsp;John B. Claridge ,&nbsp;Alexandros P. Katsoulidis ,&nbsp;Matthew J. Rosseinsky","doi":"10.1016/j.apcata.2025.120308","DOIUrl":"10.1016/j.apcata.2025.120308","url":null,"abstract":"<div><div>The catalytic selective oxidation of biomass-derived platform chemicals into monomers offers a sustainable alternative pathway to fossil-based production of chemicals. Herein, mesoporous Al<sub>2</sub>O<sub>3</sub> with dispersed Mo-V oxide catalysts were prepared through a solvent-free solid-state grinding method for the liquid phase oxidation of furfural to maleic anhydride. The selective oxidation of furfural to maleic anhydride was dependent on the Mo/V mole ratio of the catalyst, catalyst calcination temperature, and catalyst synthesis method. The synergistic interaction of Mo-V with Al<sub>2</sub>O<sub>3</sub> was identified as crucial for enhancing catalytic activity and selectivity towards maleic anhydride. The reusability of the 25Mo<sub>1</sub>VA catalyst was studied over five catalytic cycles with a progressive loss of maleic anhydride yield due to the formation of surface carbonaceous species. However, the majority of maleic anhydride yield could be recovered utilizing a catalyst regeneration cycle (600 °C, 3 h).</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"700 ","pages":"Article 120308"},"PeriodicalIF":4.7,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143874145","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Adsorption of Al2O3 {100} hydroxyl and Ni-Al2O3 electron transfer synergetic catalysis for efficient selective hydrogenation of unsaturated aldehydes Al2O3{100}羟基吸附与Ni-Al2O3电子转移协同催化不饱和醛的高效选择性加氢
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-22 DOI: 10.1016/j.apcata.2025.120306
Tianyi Huang , Jiajia Wu , Yongqi Pan , Zhiyuan Yu , Fangyu Zhao , Shafqat Ullah , Yang Xu , Yong Chen , Zhehao Sun , Zongyou Yin , Qiangqiang Xue , Sibudjing Kawi , Shuliang Lu , Yujun Wang , Guangsheng Luo
{"title":"Adsorption of Al2O3 {100} hydroxyl and Ni-Al2O3 electron transfer synergetic catalysis for efficient selective hydrogenation of unsaturated aldehydes","authors":"Tianyi Huang ,&nbsp;Jiajia Wu ,&nbsp;Yongqi Pan ,&nbsp;Zhiyuan Yu ,&nbsp;Fangyu Zhao ,&nbsp;Shafqat Ullah ,&nbsp;Yang Xu ,&nbsp;Yong Chen ,&nbsp;Zhehao Sun ,&nbsp;Zongyou Yin ,&nbsp;Qiangqiang Xue ,&nbsp;Sibudjing Kawi ,&nbsp;Shuliang Lu ,&nbsp;Yujun Wang ,&nbsp;Guangsheng Luo","doi":"10.1016/j.apcata.2025.120306","DOIUrl":"10.1016/j.apcata.2025.120306","url":null,"abstract":"<div><div>The hydrogenation of the C<img>C bond in α-β unsaturated aldehydes faces substantial difficulties due to the steric hindrance and the conjugation effects of macromolecular unsaturated aldehydes. Herein, we introduce a novel approach to prepare nanosheet-structured Ni-Al<sub>2</sub>O<sub>3</sub> catalysts featuring exposed {100} crystal planes and hydroxyl groups, utilizing a microfluidic system to easily control crystal plane growth achieve support modification. In-situ characterizations and DFT calculations reveal that the exposed {100} crystal plane, a strong metal-support interaction (SMSI) promotes electron transfer of Ni and significantly reducing the C<img>C hydrogenation energy barrier from 3.12 eV to 1.79 eV. The hydroxyl environment facilitates effective adsorption of the C<img>O bond, accelerating the reaction and enabling rapid desorption of the product. Under modified reaction conditions for the preparation of 2-ethylhexanol, the catalyst still achieved a yield of 99.9 %. This simple method of support modification enables rapid large-scale preparation, possessing significant potential for industrial applications.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"700 ","pages":"Article 120306"},"PeriodicalIF":4.7,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143868544","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Design of platinum group metal-free automotive three-way catalyst: MgMn2O4 and CuCo2O4 in tandem layout MgMn2O4和CuCo2O4串联布局无铂族金属汽车三元催化剂的设计
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2025-04-21 DOI: 10.1016/j.apcata.2025.120305
Keisuke Maruichi , Taichi Yamaguchi , Ryosuke Sakai , Kakuya Ueda , Akira Oda , Atsushi Satsuma
{"title":"Design of platinum group metal-free automotive three-way catalyst: MgMn2O4 and CuCo2O4 in tandem layout","authors":"Keisuke Maruichi ,&nbsp;Taichi Yamaguchi ,&nbsp;Ryosuke Sakai ,&nbsp;Kakuya Ueda ,&nbsp;Akira Oda ,&nbsp;Atsushi Satsuma","doi":"10.1016/j.apcata.2025.120305","DOIUrl":"10.1016/j.apcata.2025.120305","url":null,"abstract":"<div><div>Platinum group metal (PGM)-free and Cr-free automotive three-way catalyst (TWC) was examined using two types of base-metal oxides for hydrocarbon preferential oxidation (HC-PROX) and NO reduction by CO in tandem configuration. MnOx-based binary mixed metal oxides (X1Mn2, X = Ba, Ca, Co, Cu, Fe, Mg, Ni, Zn, Zr) were investigated for the design of HC-PROX catalysts. Mg1Mn2 achieved both high propene oxidation activity and low CO oxidation activity, and the catalyst phase was determined as MgMn<sub>2</sub>O<sub>4</sub> having the spinel structure. A tandem TWC composed of MgMn<sub>2</sub>O<sub>4</sub> for HC-PROX and CuCo<sub>2</sub>O<sub>4</sub> for NO-CO reaction showed comparable NO reduction activity and higher oxidation activity of propene and CO compared to Rh/ZrO<sub>2</sub> as a benchmark. In-situ FTIR study clarified that the suppression of CO oxidation over MgMn<sub>2</sub>O<sub>4</sub> is caused by strongly adsorbed acetate and formate on the catalyst surface.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"700 ","pages":"Article 120305"},"PeriodicalIF":4.7,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143855003","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
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