Applied Catalysis A: General最新文献_第10页

Planer type solid oxide cells using La0.9Sr0.1Ga0.8Mg0.2O3-δ thin-film electrolyte prepared by dip-coating method for high performance CO2/H2O co-electrolysis

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-02-02 DOI: 10.1016/j.apcata.2025.120146

Longtai Li , Motonori Watanabe , Miki Inada , Tatsumi Ishihara

{"title":"Planer type solid oxide cells using La0.9Sr0.1Ga0.8Mg0.2O3-δ thin-film electrolyte prepared by dip-coating method for high performance CO2/H2O co-electrolysis","authors":"Longtai Li , Motonori Watanabe , Miki Inada , Tatsumi Ishihara","doi":"10.1016/j.apcata.2025.120146","DOIUrl":"10.1016/j.apcata.2025.120146","url":null,"abstract":"<div><div>Ni-Zr0.92Y0.16O2.08(YSZ)-supported solid oxide cell with La0.9Sr0.1Ga0.8Mg0.2O3-δ(LSGM) thin film as the electrolyte was prepared with dip-coating and co-sintering methods. CO2/H2O co-electrolysis and CO2 electrolysis performance were studied. Initial performance measurement from 1073 to 773 K shows reasonably high open circuit voltage (OCV) with superior current densities, particularly in CO2/H2O co-electrolysis, up to −4.9 A/cm2 at 1073 K and −0.19 A/cm2 at 773 K. Product analysis suggests that H2 and CO production was attributed to both electrolysis and the reverse water-gas shift (RWGS) reaction, with almost 100 % Faraday efficiency. The H2/CO ratio in the product ranged from 1.4 to 1.5 in co-electrolysis when CO2/H2O= 1/1 gas was fed. Performance comparison at 1073 K indicated that direct CO2 electrolysis occurred, however, steam electrolysis predominately occurred under co-electrolysis conditions. The prepared cell shows good stability at −0.1 A/cm2 under CO2/H2O co-electrolysis for 200 h, with almost no change in terminal potential with minimal degradation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"694 ","pages":"Article 120146"},"PeriodicalIF":4.7,"publicationDate":"2025-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143369449","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

Rigid Na-OH ionic-bond framework in the Helmholtz layer induces the kinetic pH effect in hydrogen electrocatalysis on Pt

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-01-30 DOI: 10.1016/j.apcata.2025.120148

Min Ouyang , Shaoyu Kong , Wei Cao , Dongxue Zhang, Feipeng Zheng, Xiaobo Chen

{"title":"Rigid Na-OH ionic-bond framework in the Helmholtz layer induces the kinetic pH effect in hydrogen electrocatalysis on Pt","authors":"Min Ouyang , Shaoyu Kong , Wei Cao , Dongxue Zhang, Feipeng Zheng, Xiaobo Chen","doi":"10.1016/j.apcata.2025.120148","DOIUrl":"10.1016/j.apcata.2025.120148","url":null,"abstract":"<div><div>A large challenge in hydrogen electrocatalysis is the great decrease in catalytic activity of noble metals when moving from acidic electrolytes to basic ones. Based on first-principles calculations, we report that the Pt/electrolyte interface undergoes a transformation from a highly mobile hydrogen-bond network of water in acid to a solid-state and rigid Na-OH ionic-bond framework in base. Meanwhile, the hydrogen coverage decreases from 100 % to 16 %. This transformation leads to a barrierless water dissociation process, challenging the traditional belief that water splitting is the primary obstacle. The solid-state NaOH layer impedes proton migration towards the interface and retards hydrogen desorption, resulting in the sluggish kinetics. Incorporation of Ni atoms at the interface builds a proton transfer channel through the NaOH layer, enhancing the proton transfer kinetics. We suggest that electron-donor dopants can enhance the kinetics of both the interfacial reactions and the proton transfer in solution.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"694 ","pages":"Article 120148"},"PeriodicalIF":4.7,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143162744","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

Highly dispersed Fe in P dopped N-C for the catalytic peroxidation of 1,3-diisopropylbenzene with molecular oxygen

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-01-30 DOI: 10.1016/j.apcata.2025.120147

Shikai Wang , Yafan Wang , Fei Zha , Xiaohua Tang , Yue Chang , Haifeng Tian

{"title":"Highly dispersed Fe in P dopped N-C for the catalytic peroxidation of 1,3-diisopropylbenzene with molecular oxygen","authors":"Shikai Wang , Yafan Wang , Fei Zha , Xiaohua Tang , Yue Chang , Haifeng Tian","doi":"10.1016/j.apcata.2025.120147","DOIUrl":"10.1016/j.apcata.2025.120147","url":null,"abstract":"<div><div>The decomposition of 1,3-diisopropylbenzene dihydroperoxide (DHP) obtained by the catalytic oxidation of 1,3-diisopropylbenzene (DIPB) is known as the main industrial process to produce resorcinol. A new catalyst of highly dispersed Fe in P-doped N-C (Fe-N/P-C) was synthesized using a ligand-assisted method, and was applied for the peroxidation of DIPB. SEM, TEM and HAADF-STEM revealed that Fe is uniformly dispersed on N/P-C. XRD, Raman spectra, N2 adsorption/desorption, XPS and O2-TPD showed that doping of P species in N-C leads to form more mesopore and increases the disorder degree, providing more active sites for the activation of tertiary C-H bonds in DIPB. The conversion of DIPB was 97.8 % and the yield of DHP was 67.2 % under mass of Fe-N/P-C to DIPB was 1.0, reaction temperature was 90°C, oxygen flow rate was 100 mL/min, and reaction time was 8 h. The investigation of radical quenching and mass spectrometry suggested that the increased oxidation rate is attributed to the involvement of Fe-N/P-C in both chain initiation and chain propagation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"694 ","pages":"Article 120147"},"PeriodicalIF":4.7,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143378049","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

Ag-decorated Cu2O porous hollow catalyst for promoting CO2 electroreduction to C2H4 via enrichment of CO

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-01-28 DOI: 10.1016/j.apcata.2025.120145

Jianhao Li, Zhicheng Hu, Shuhuan Han, Dapeng Cao, Xiaofei Zeng, Jianfeng Chen

{"title":"Ag-decorated Cu2O porous hollow catalyst for promoting CO2 electroreduction to C2H4 via enrichment of CO","authors":"Jianhao Li, Zhicheng Hu, Shuhuan Han, Dapeng Cao, Xiaofei Zeng, Jianfeng Chen","doi":"10.1016/j.apcata.2025.120145","DOIUrl":"10.1016/j.apcata.2025.120145","url":null,"abstract":"<div><div>Electrocatalytic CO2 reduction reaction (CO2RR) to multi-carbon product, especially for ethylene (C2H4), provides a favorable pathway for carbon neutrality and renewable energy storage. However, the second-order C-C coupling reactions in CO2RR need always the high activation/driven energy in dynamics originating from the trace C1 intermediate product. Herein, we synthesized the Ag-decorated Cu2O porous hollow core-shell catalyst named Ag@Cu2O where Ag nanoparticles uniformly distributed on inner the surface of the hollow Cu2O (H-Cu2O) via the sacrificial template method. Benefiting from the synergistic hollow structure and electron transfer from Cu and Ag to O, Ag@Cu2O catalyst delivers the excellent C2H4 Faradaic Efficiency (FE) of 55 % ± 2 % at −1.0 V (vs. RHE), which is superior to the most reported catalysts. More importantly, in situ infrared spectroscopy and density functional theory (DFT) calculations reveal the introduction of Ag can decrease the activation energy required for *CO and C-C coupling.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"694 ","pages":"Article 120145"},"PeriodicalIF":4.7,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143163857","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

Roles of NOx and the supported RuO2 in accelerating soot oxidation over RuO2/CeO2–ZrO2

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-01-28 DOI: 10.1016/j.apcata.2025.120144

Hitoshi Kubo , Yusuke Ohshima , Shunsuke Kato , Noriyuki Saitoh , Noriko Yoshizawa , Osamu Nakagoe , Shuji Tanabe

{"title":"Roles of NOx and the supported RuO2 in accelerating soot oxidation over RuO2/CeO2–ZrO2","authors":"Hitoshi Kubo , Yusuke Ohshima , Shunsuke Kato , Noriyuki Saitoh , Noriko Yoshizawa , Osamu Nakagoe , Shuji Tanabe","doi":"10.1016/j.apcata.2025.120144","DOIUrl":"10.1016/j.apcata.2025.120144","url":null,"abstract":"<div><div>RuO2/CeO2–ZrO2 (Ru/CZ) shows high activity for soot oxidation in a NO2/O2 flow. The soot oxidation occurred at the soot-Ru/CZ interface and at the soot surface. It was shown that RuO2 increases the Ce3 +/Ce in CZ surface, and that dissociates the adsorbed O2 and supplies O atoms to CZ support. Adsorbed-NO3 (ad-NO3) contributed more than gaseous NO2 to soot oxidation. The investigation of activation energy and outlet NOx gas suggested that ad-NO3 ignited soot, and then CZ lattice oxygen and reactive oxygen species derived from CZ support mainly oxidized soot. Although the molar ratio of ad-NO3/soot was only 1 %, ad-NO3 accelerated soot oxidation. This was implied to be because ad-NO3 oxidizes soot through the redox cycle between ad-NO2 and ad-NO3 by CZ lattice oxygen. Soot oxidation over Ru/CZ is believed to be accelerated by the synergistic effect of the O2 dissociation by RuO2 and the ignition of soot by ad-NO3.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"693 ","pages":"Article 120144"},"PeriodicalIF":4.7,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143099824","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

Photo-driven metal-free radical addition reaction for the degradation of formaldehyde polymers

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-01-27 DOI: 10.1016/j.apcata.2025.120143

Sheng Bi , Qiangwei Li , Le-Cheng Wang , Xiao-Feng Wu

引用次数: 0

Inverse opal type porous g-C3N4 towards H2O2 production and in-situ photoFenton gemifloxacin degradation driven by amorphous framework and nitrogen vacancy

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-01-27 DOI: 10.1016/j.apcata.2025.120141

Sriram Mansingh , Kundan Kumar Das , Ritik Mohanty , Newmoon Priyadarshini, Kulamani Parida

{"title":"Inverse opal type porous g-C3N4 towards H2O2 production and in-situ photoFenton gemifloxacin degradation driven by amorphous framework and nitrogen vacancy","authors":"Sriram Mansingh , Kundan Kumar Das , Ritik Mohanty , Newmoon Priyadarshini, Kulamani Parida","doi":"10.1016/j.apcata.2025.120141","DOIUrl":"10.1016/j.apcata.2025.120141","url":null,"abstract":"<div><div>H2O2 production by utilizing renewable feedstocks like solar energy, H2O and O2 through artificial photocatalysis is an intriguing area of sustainable research. Porous and defect-oriented g-C3N4 is a promising metal free material for photon driven H2O2 generation via. O2/H2O redox pathway because of its benefitting features. The designed vacancy-oriented carbon nitride with amorphous character along with inverse opal type framework boost the overall O2 reduction rate and on-situ gemifloxacine (GFM) degradation. The PCN sample manifest the optimum peroxide generation (587 µmol/g/h and conversion efficiency of 0.011 %) which is 1.4 times higher than CN. The photoreduction goes predominantly via. both single electron two step, i.e., ●O2- radical route confirms by scavenger and EPR test. Further, reduction reaction was also evaluated under different reaction condition, i.e., pH, sacrificial agent and purging gas type. Besides, PCN depicts enhanced onsite photo-fenton GFM degradation (78 % in 1 h) and the formed intermediates species alongside the mineralization 70 % is well demonstrated. This investigation serves as a guideline for the development of different amorphous and defect based photocatalysts for sustainable H2O2 generation and on-site photo-fenton activity with benchmark efficiency</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"693 ","pages":"Article 120141"},"PeriodicalIF":4.7,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143099823","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

Enhanced stability and activity in the upgrading ethanol to n-butanol using a ruthenium polyphenylene catalyst

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-01-27 DOI: 10.1016/j.apcata.2025.120139

Xuetong Pei , Mengyao Su , Christopher Waldron , Marc Walker , Donato Decarolis , Qian He , Stuart Archer , Martin B. Smith , Sandra E. Dann , Simon A. Kondrat

{"title":"Enhanced stability and activity in the upgrading ethanol to n-butanol using a ruthenium polyphenylene catalyst","authors":"Xuetong Pei , Mengyao Su , Christopher Waldron , Marc Walker , Donato Decarolis , Qian He , Stuart Archer , Martin B. Smith , Sandra E. Dann , Simon A. Kondrat","doi":"10.1016/j.apcata.2025.120139","DOIUrl":"10.1016/j.apcata.2025.120139","url":null,"abstract":"<div><div>Bioethanol upgrading to n-butanol is catalysed by homogeneous catalysts under mild solventless liquid phase conditions, at which heterogeneous catalysts have poor performance. Here a heterogeneous catalyst, initially comprised of a Ru(bipy) complex incorporated into a polyphenylene support, gave a catalytic performance (TON of 3565 Ru−1 and 82 % n-butanol selectivity) that exceeded contemporary homogeneous and heterogeneous catalysts. Catalyst deactivation by water byproduct inhibition was improved by removal of water, via recharging the reactor with fresh ethanol, or by the co-addition of molecular sieve. The Ru polyphenylene catalyst showed greater stability in the presence of molecular sieve compared to the homogeneous catalyst, enabling high butanol yields. Characterisation showed a structural transformation of the single atom Ru(bipy) into 2.6 nm Ru(0) nanoparticles after 16 h reaction. While the Ru(0) had moderate recyclability (TON of 1000 Ru−1) the initial highly active species seen in the fresh catalyst are not stable.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"694 ","pages":"Article 120139"},"PeriodicalIF":4.7,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143162743","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Optimizing CuNi catalysts for long-term vapor phase hydrogenation of levulinic acid to γ-valerolactone: Influence of the support on activity and stability

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-01-27 DOI: 10.1016/j.apcata.2025.120140

Eliana Quiroga , Bernay Cifuentes , Santiago Yara , Julia Moltó , Martha Cobo

{"title":"Optimizing CuNi catalysts for long-term vapor phase hydrogenation of levulinic acid to γ-valerolactone: Influence of the support on activity and stability","authors":"Eliana Quiroga , Bernay Cifuentes , Santiago Yara , Julia Moltó , Martha Cobo","doi":"10.1016/j.apcata.2025.120140","DOIUrl":"10.1016/j.apcata.2025.120140","url":null,"abstract":"<div><div>The conversion of biomass-derived levulinic acid (LA) to γ-valerolactone (GVL) is crucial for sustainable chemical and fuel production. This study evaluates the vapor phase hydrogenation of LA using Cu-Ni bimetallic catalysts supported on various metal oxides and their impact on the pathways of LA conversion. Specifically, we examine the influence of AlO2, SiO2, ZrO2-SiO2, and CeO2-SiO2 on catalyst performance and stability. Cu-Ni catalysts supported on SiO2 modified with citric acid (SiO2-CA) exhibited superior stability, while the one supported on Al2O3 showed higher activity. The enhanced performance of the SiO2-CA-supported catalyst is attributed to its moderate acidity (379.3 µmol/gcat) and resistance to sintering. Stability tests reveal that although both CuNi/Al2O3 and CuNi/SiO2-CA catalysts deactivate over time, the latter demonstrates slower deactivation and better reactivation potential, maintaining conversion close to 80 % for 42 h. The study highlights the role of support in optimizing catalytic performance for LA hydrogenation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"694 ","pages":"Article 120140"},"PeriodicalIF":4.7,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143163856","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Transalkylation between C10 aromatics and 2-methylnaphthalene to synthesize 2,6-dimethylnaphthalene by Mo-modified HZSM-12 catalysts

IF 4.7 2区化学

Applied Catalysis A: General Pub Date : 2025-01-27 DOI: 10.1016/j.apcata.2025.120138

Cheng Xiong , Shuai Meng , Runping Ye , Huibing Shi , Deming Zhao , Rongbin Zhang , Gang Feng

{"title":"Transalkylation between C10 aromatics and 2-methylnaphthalene to synthesize 2,6-dimethylnaphthalene by Mo-modified HZSM-12 catalysts","authors":"Cheng Xiong , Shuai Meng , Runping Ye , Huibing Shi , Deming Zhao , Rongbin Zhang , Gang Feng","doi":"10.1016/j.apcata.2025.120138","DOIUrl":"10.1016/j.apcata.2025.120138","url":null,"abstract":"<div><div>Zeolites are important catalysts for the synthesis of 2,6-dimethylnaphthalene (2,6-DMN) by the raw materials of 2-methylnaphthalene (2-MN) and C10 aromatics. However, the selectivity of 2,6-DMN is still difficult to control and the catalysts often suffer from poor hydrothermal stability. In this work, a series of Mo-modified HZSM-12 catalysts were prepared and investigated for the transalkylation reaction between 2-MN and C10 aromatics under a hydrogen atmosphere. The introduction of Mo binds to the B-acid sites on the molecular sieves, modulating the B-acid strength and content of the catalysts while also altering their pore structure. As a result, the 3 %Mo/HZSM-12 catalyst exhibited excellent catalytic performance, the conversion of 2-MN could still reach up to 61.3 % and the ratio of 2,6-/2,7-DMN was able to reach 1.69 after 6 h of the reaction. Therefore, our work is expected to provide a useful strategy for constructing efficient zeolite catalysts for the synthesis of high-value esters’ precursors.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"693 ","pages":"Article 120138"},"PeriodicalIF":4.7,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143099877","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