Applied Catalysis A: General最新文献

{"title":"Charge separation engineering: The synergistic effect of oxidation half-reaction and reduction half-reaction to promote photocatalytic hydrogen production","authors":"Cheng Yang,&nbsp;Xiaolong Ma,&nbsp;Zhiliang Jin","doi":"10.1016/j.apcata.2025.120381","DOIUrl":"10.1016/j.apcata.2025.120381","url":null,"abstract":"<div><div>With a view to effectively promote the spatial separation ability of photogenerated carriers, designing photocatalysts and photocatalytic systems with high-efficient charge separation ability is an effective strategy to solve the problem of low carrier separation efficiency in the light-induced process. The composite photocatalyst UPC-HOF-6/Mn₂O₃/Pt with high-efficient charge separation ability is designed by anchoring Mn₂O₃ with oxidation ability and Pt with reduction ability to the oxidation site and reduction site respectively, achieving the rapid separation of photogenerated electron-hole pairs. Through the analysis of electron paramagnetic resonance technology, the charge transfer direction of the composite photocatalyst under light irradiation is clarified. The hydrogen evolution activity of the optimized composite photocatalyst UPC-HOF-6/Mn₂O₃/Pt is 6574.9 μmol·g⁻¹, which is 6574.9 times and 206.9 times that of UPC-HOF-6 (0 μmol g⁻¹) and Mn₂O₃ (31.7 μmol g⁻¹) respectively, showing excellent photocatalytic activity. The realization of the rapid separation of photogenerated electron-hole pairs by designing photocatalysts with high-efficient charge separation ability lays a theoretical foundation for improving the spatial separation ability of photogenerated carriers.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120381"},"PeriodicalIF":4.7,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144169024","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}

{"title":"Oxidation of n-alkanes using TS-1 and H2O2: Effects of chain length and solvents","authors":"Seyeon Park ,&nbsp;Maura Gibbs ,&nbsp;Zhuoming Feng ,&nbsp;Karen I. Goldberg ,&nbsp;Daeyeon Lee ,&nbsp;Raymond J. Gorte ,&nbsp;John M. Vohs","doi":"10.1016/j.apcata.2025.120378","DOIUrl":"10.1016/j.apcata.2025.120378","url":null,"abstract":"<div><div>The selective oxidation of n-C₈H₁₈, n-C₁₂H₂₆, n-C₁₆H₃₄, n-C₂₀H₄₂, and n-C₃₆H₇₄ was studied with a goal of using these as models to provide insight into how to functionalize polyolefins. Reactions were carried out using a TS-1 catalyst and H₂O₂ in a batch reactor with different cosolvents, including methanol, acetone, acetonitrile, methyl ethyl ketone, and methyl butyl ketone. Rates decreased with increasing alkane size, possibly due to the reduced solubility of larger alkanes into the water-rich phases. Cosolvents that promote the partitioning of alkanes in the aqueous phase increased the rates. ¹H NMR spectroscopy demonstrated that ketones were the primary products, although some alcohols also formed. There was preferential reaction at the 2 position in the alkanes, but reaction at central carbons was also observed. The results of this study suggest strategies for using this catalytic chemistry to functionalize polyolefins.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120378"},"PeriodicalIF":4.7,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144169022","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}

{"title":"Mechanism exploration of Cu-SnS2-sv@GO during the process of converting cellulose hydrolysate to lactic acid under mild reaction conditions","authors":"Pingli Sun ,&nbsp;Xinrui Wang ,&nbsp;Shaocong Yang ,&nbsp;Fanyao Meng ,&nbsp;Yue Zhao ,&nbsp;Xiaomeng Zhou ,&nbsp;Jianing Wang ,&nbsp;Xinjian Zhang ,&nbsp;Zhen Wang","doi":"10.1016/j.apcata.2025.120371","DOIUrl":"10.1016/j.apcata.2025.120371","url":null,"abstract":"<div><div>Valorization of cellulose-based materials requires overcoming the energy barrier of glucose isomerization to fructose. However, the process is often reliant on high temperatures and harsh thermal-catalytic conditions. In this study, 6 %Cu-SnS_2-sv@GO aerogels were developed as catalysts to produce lactic acid (LA) from enzyme-pretreated microcrystalline cellulose. These aerogels demonstrated remarkable thermo-catalytic and photocatalytic performances. The participation of Cu significantly enhanced the Lewis acidity and the total acidity of the catalyst, thereby boosting thermo-catalytic efficiency. Notably, the catalyst facilitated glucose isomerization to fructose at relatively low temperatures, with the reaction launching around 40 °C. Furthermore, Cu doping modulates the band structure of the catalyst, enhancing its light absorbability and improving the separation efficiency of photoinduced electron-hole pairs. Fructose produced during the single thermo-catalysis process accumulates due to its slow conversion rate. In contrast, the accumulated fructose is effectively depleted during thermo-photocatalysis, significantly enhancing both the selectivity and yield of levulinic acid (LA). Among the synthesized catalysts, 6 %Cu-SnS_2-sv@GO demonstrated the highest performance, achieving an optimal LA yield of 83.6 % (based on the enzymatic hydrolysate) at 80 °C under 2 hours of visible-light irradiation. These findings present a novel and efficient strategy for the high-value utilization of cellulose-based materials.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120371"},"PeriodicalIF":4.7,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144147953","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}

{"title":"Hydrophilic porous organic polymers with fluorene-viologen units for enhanced photocatalytic hydrogen production","authors":"Sinem Altınışık ,&nbsp;Gizem Yıldız ,&nbsp;Kübra Turgut ,&nbsp;Cansu Yayla ,&nbsp;İmren Hatay Patır ,&nbsp;Sermet Koyuncu","doi":"10.1016/j.apcata.2025.120377","DOIUrl":"10.1016/j.apcata.2025.120377","url":null,"abstract":"<div><div>The rising energy demand and environmental concerns have intensified the search for clean energy solutions. Photocatalytic water splitting offers a promising route, yet efficiency remains limited by the need for advanced photocatalysts with enhanced light absorption, charge separation, and water interaction. Porous organic polymers (POPs) are emerging as efficient materials for solar energy conversion due to their ordered conjugated structures. This study explores the impact of a ketone moiety on the hydrophilicity and photocatalytic hydrogen evolution efficiency of fluorene-bridged bicarbazole-viologen-based POPs (POP-MB-TP(DCzFO) and POP-MB-TP(DCzF)). Our results show that POP-MB-TP(DCzF) achieves a hydrogen evolution rate of 3.37 mmol g⁻¹ h⁻¹, nearly twice that of POP-MB-TP(DCzFO) (1.72 mmol g⁻¹ h⁻¹). This improvement highlights the role of hydrophilicity in charge transport and catalytic efficiency, providing insights for designing highly efficient organic photocatalysts for sustainable hydrogen production.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120377"},"PeriodicalIF":4.7,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144169021","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}

{"title":"Modification of Bi2WO6 containing oxygen vacancies with Au to promote selective oxidation of benzyl alcohol","authors":"Kaiyi Sun,&nbsp;Tinglan Wang,&nbsp;Ting Shang,&nbsp;Hongjie Wang,&nbsp;Guilan Fan,&nbsp;Wenyan Zhao,&nbsp;Jingyi Li","doi":"10.1016/j.apcata.2025.120376","DOIUrl":"10.1016/j.apcata.2025.120376","url":null,"abstract":"<div><div>Selective oxidation of benzyl alcohol to benzaldehyde by photocatalytic technology is important in the synthesis of pharmaceuticals and fine chemicals. Here, we prepared oxygen vacancy-containing Bi₂WO₆ (Bi₂WO₆-Ov) as a precursor by hydrothermal method, and prepared 2 wt% Au/Bi₂WO₆-Ov by sodium borohydride reduction method. 2 wt% Au/Bi₂WO₆-Ov dramatically upgraded the photocatalytic performance (The conversion of benzyl alcohol was 93.8 %) by utilizing the oxygen vacancy and the low loading of Au, which is nearly 10 times higher than that of conventional Bi₂WO₆-Ov. A series of characterization results (XRD, XPS, UV–vis DRS, PL, SEM, TEM, etc.), combined with DFT calculations, revealed that benzyl alcohol was well adsorbed on Au NPs (nanoparticles) as an acidic site, and the oxygen vacancies acted as an electron bridge and acted as Lewis bases. The electrons were transferred from the surface of Bi₂WO₆-Ov to Au, upgrading the electron-hole separation efficiency, which raised the ability of benzyl alcohol oxidation. Based on the above experiments and DFT calculations, a possible mechanism is proposed.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120376"},"PeriodicalIF":4.7,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144147952","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}

{"title":"Ga-SrTiO3 modified by CuCrOx/Co3O4 dual cocatalyst for efficient photocatalytic overall water splitting","authors":"Yiquan Zhan ,&nbsp;Shaohui Lai ,&nbsp;Junzhe Jiang ,&nbsp;Lijiao Zhong ,&nbsp;Yongsheng Liu ,&nbsp;Kai Yang ,&nbsp;Jinbiao Liu ,&nbsp;Shiyong Liu ,&nbsp;Liqing Li ,&nbsp;Yoshihisa Sakata","doi":"10.1016/j.apcata.2025.120373","DOIUrl":"10.1016/j.apcata.2025.120373","url":null,"abstract":"<div><div>Strontium titanate (SrTiO₃) holds great potential for photocatalytic overall water splitting (OWS) to produce hydrogen. However, the current SrTiO₃-based photocatalysts require expensive noble metals, such as Pt and Rh. There is an urgent need to explore cost-effective alternatives using non-noble metals. Herein, Cu, Cr, and Co were used as non-noble cocatalyst to modify the surface of Ga˗doped SrTiO₃ photocatalyst (Ga-STO (flux)). The characterization results of XPS and TEM revealed the CuCrO_<em>x</em> cocatalysts generated reduced Cu⁰/Cu⁺ species for hydrogen evolution reaction. The inclusion of Cr₂O₃ aided in maintaining the stability of Cu⁰/Cu⁺ species. The Co₃O₄ cocatalysts were responsible for the oxygen evolution reaction. Under simulated sunlight, the optimal CuCrO_<em>x</em>/Co₃O₄/Ga-STO (flux) sample provided the best hydrogen and oxygen production rates of 204.56 μmol·h⁻¹ and 102.28 μmol·h⁻¹ , respectively.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120373"},"PeriodicalIF":4.7,"publicationDate":"2025-05-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144147954","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}

{"title":"Boosting catalytic activity of Ag-modified CeO2-Al2O3 mixed metal oxide support via coupling with a VUV photoreactor: A catalytic ozonation system applied towards VOC oxidation","authors":"Amir Payan,&nbsp;Farid Jafarihaghighi,&nbsp;Jafar Soltan","doi":"10.1016/j.apcata.2025.120370","DOIUrl":"10.1016/j.apcata.2025.120370","url":null,"abstract":"<div><div>This study introduces a new air purification strategy that combines a vacuum ultraviolet (VUV) photoreactor as an in-situ source of O₃ generation coupled with a fixed-bed ozonation reactor equipped with Ag-based catalysts. The results showed that the integration of the VUV photoreactor to the fixed-bed reactor significantly enhanced not only the conversion of acetone but also improved the O₃ decomposition compared to the catalytic ozonation system alone in that the acetone and O₃ conversion were boosted from 82 % and 86 %, respectively, to 100 % each. While the inhibitory impact of relative humidity (RH) on Ag/CeO₂−Al₂O₃ activity using a fixed bed reactor was detected, coupling with the VUV photoreactor led to maintaining 100 % conversion of acetone and ozone even in the humid condition. Indeed, although RH poisoned the interface of the gas-catalyst, leading to an inhibition role in the catalytic reactions, it improved the VUV photolysis performance in the gaseous state, resulting in the enhancement of the coupled reactor’s performance compared to the only catalytic ozonation fixed bed reactor. Additionally, the in-situ regeneration capability, which was introduced to the air treatment system by combining the VUV photoreactor with the traditional catalytic ozonation, granted prolonged reusability of the catalyst with minimal activity reduction (less than 2 %). The attained data showed that the presence of binary metal oxide supports with an optimized 1:1 ratio had a key role in maintaining not only a complete conversion of acetone and ozone but also achieving above 99 % reaction selectivity towards complete oxidation. Finally, a mechanistic study was conducted where the in-situ diffuse reflectance infrared Fourier transform (DRIFT) analysis proved the role of surface carboxylate and electron paramagnetic resonance (EPR) data demonstrated the co-participation of ^{<strong>.</strong>}OH/^{<strong>.</strong>}O₂⁻ radicals in acetone removal.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"704 ","pages":"Article 120370"},"PeriodicalIF":4.7,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144169023","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}

{"title":"Nitrogen-oxygen defects polytriazineimide photocatalytic efficient and selective oxidation of benzyl alcohol","authors":"Meiting Song ,&nbsp;Zhenglong Shen ,&nbsp;Ying Liu ,&nbsp;Yiguo Su ,&nbsp;Yuhang Wu","doi":"10.1016/j.apcata.2025.120368","DOIUrl":"10.1016/j.apcata.2025.120368","url":null,"abstract":"<div><div>By a one-step molten salt calcination method, the copolymer 4,6-diaminopyrimidine was successfully incorporated into the precursor melamine to prepare a polytriazineimide photocatalyst rich in nitrogen and oxygen defects for the selective oxidation of benzyl alcohol. A series of characterizations confirmed the existence of the defects, and the photoelectric performance test showed that the defects could enhance the responsiveness of the catalyst to light and facilitate the separation of photogenerated carriers. Moreover, the existence of nitrogen and oxygen defects helps to adsorb more surface oxygen molecules to generate more superoxide radicals as the main active species to selectively oxidize benzyl alcohol. Therefore, the 46DP-10 % sample exhibits excellent benzyl alcohol oxidation performance, the conversion rate is 84.9 % under visible light oxygen atmosphere, and the selectivity is greater than 99 %. This work presents a novel idea for creating nitrogen and oxygen deficient materials through molten salt-assisted calcination of precursors and copolymers.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120368"},"PeriodicalIF":4.7,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144131341","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}

{"title":"Metal-Salphen covalent organic polymers for bifunctional electrocatalytic ammonia synthesis and oxygen evolution","authors":"Jiani Zhao ,&nbsp;Yuhan Xia ,&nbsp;Wenhua Xu,&nbsp;You Lv,&nbsp;Chengbo Li,&nbsp;Jun Li,&nbsp;Ning Wang","doi":"10.1016/j.apcata.2025.120369","DOIUrl":"10.1016/j.apcata.2025.120369","url":null,"abstract":"<div><div>Herein, we report a one-pot synthesis of metal-salphen-based covalent organic polymers (MSalphen-COPs) through Schiff base condensation of 1,3,5-triformylphloroglucinol and o-phenylenediamine in the presence of M(OAc)₂·nH₂O (M = Co, Ni, Cu). FTIR spectra confirm the successful formation of COPs via imine condensation while revealing an irreversible enol-keto tautomerization process that drives the structural evolution toward a thermodynamically stabilized framework. XPS analyses reveal that metal ions coordinate with deprotonated amine nitrogen and carbonyl oxygen moieties, deviating from conventional imine nitrogen/phenolate oxygen coordination in Metal-Salphen complexes. The electrocatalytic performance of MSalphen-COPs for nitrate/nitrite reduction (NO_xRR) and oxygen evolution reaction (OER) exhibits strong metal-dependent trends, with CoSalphen-COP achieving exceptional activity. DFT calculations attribute cobalt’s superiority to its lowest barriers along catalytic cycles. Leveraging its bifunctionality, a CoSalphen-COP-based NO₃RR||OER system demonstrates efficient NH₃/O₂ coproduction, validating its potential for sustainable electrochemical applications. This work establishes a paradigm for designing task-specific COPs through tailored metal-ligand coordination environments.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120369"},"PeriodicalIF":4.7,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144124884","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}

{"title":"A comparative study proposing performance benchmarks for convoying industrial CO2-to-formate electroconversion","authors":"Jie Xiao ,&nbsp;Dong-Dong Ma ,&nbsp;Xinquan Shen ,&nbsp;Shu-Guo Han ,&nbsp;Wenbo Wei ,&nbsp;Qi-Long Zhu","doi":"10.1016/j.apcata.2025.120362","DOIUrl":"10.1016/j.apcata.2025.120362","url":null,"abstract":"<div><div>Selecting suitable electrocatalytic benchmarks can greatly enhance electrocatalyst design and better assess their performance and potential applications. However, the absence of standardized electrocatalytic benchmarks bridging laboratory innovation to industrial implementation hinders the development of pH-universal CO₂-to-formate conversion systems that meet industrial-grade current densities (&gt; 200 mA cm^–2), Faradaic efficiencies (FE &gt; 90 %), and long-term stability. Herein, through a systematic evaluation of commercial bismuth-based chemicals (metal, oxide, salts) for CO₂ electroreduction, we demonstrated that bismuth salts (e.g., Bi(NO₃)₃) as precursors for material development, can emerge as the universal performance benchmarks across all pH conditions (acidic, neutral, and alkaline). Concretely, in various electrolytic environments for formate production, these bismuth salts-coated electrodes generally exhibit exceeding 90 % FE, large current densities, low onset potentials and potential operational stability. Moreover, a comparative analysis with In/Sn/Pb analogues profoundly elucidates the general benchmarking feasibility of bismuth salts in facilitating CO₂-to-formate electroconversion. This work establishes a screening paradigm of formate-targeted electrocatalytic materials, which can assess and guide the design of practical CO₂ electrocatalysts for sustainable formate production at industrial scales.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"703 ","pages":"Article 120362"},"PeriodicalIF":4.7,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105319","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}