Molecular Catalysis最新文献

{"title":"Construction of hole transfer bridge in TiO2/β-CDP composite for photocatalytic treatment of wastewater with simultaneous hydrogen production","authors":"Hui Zhang ,&nbsp;Liuchang Yong ,&nbsp;Nan Sun ,&nbsp;Shihan Zhang ,&nbsp;Liang Zhou ,&nbsp;Fei Ke ,&nbsp;Sheng Ye","doi":"10.1016/j.mcat.2025.114911","DOIUrl":"10.1016/j.mcat.2025.114911","url":null,"abstract":"<div><div>The development of an efficient photocatalyst capable of effectively purifying wastewater while simultaneously converting solar energy into hydrogen is highly sought after, yet presents significant challenges. In this study, we developed a novel β-cyclodextrin polymer/titanium dioxide (TiO₂/β-CDP) photocatalyst exhibiting enhanced activity through a straightforward in situ sol-gel synthesis method. The TiO₂/β-CDP exhibited approximately 13.5 times greater hydrogen production compared to bare TiO₂ (162 vs. 12μmol g^-1·h^-1) during the degradation of eosin Y (EY), furthermore, upon the addition of 10 % methanol, the photocatalytic hydrogen production rate for TiO₂/β-CDP about 12 times that of TiO₂ (4415 vs. 367μmol g^-1·h^-1). The significant enhancement in photocatalytic efficiency can be attributed to the dual roles of β-CDP in this system: it serves as a matrix that promotes the heterogeneous nucleation and growth of TiO₂, and as a hole-transfer bridge that enhances charge separation. This study provides critical insights into novel biomaterials/semiconductor photocatalysts, thereby advancing their application in environmental and energy sectors.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114911"},"PeriodicalIF":3.9,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143396072","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":"Investigation of the reaction kinetics for the direct hydrogenation of maleic anhydride to 1,4-butanediol over Cu-ZnO catalyst","authors":"Xinyue Guan ,&nbsp;Yingzhe Yu ,&nbsp;Lingtao Wang ,&nbsp;Minhua Zhang","doi":"10.1016/j.mcat.2025.114908","DOIUrl":"10.1016/j.mcat.2025.114908","url":null,"abstract":"<div><div>1,4-butanediol serves as a crucial monomeric building block for the production of biodegradable plastics such as PBS and PBAT, and it can also be utilized for the synthesis of derivatives like γ-butyrolactone and tetrahydrofuran. The technology of direct hydrogenation of maleic anhydride to 1,4-butanediol over Cu-ZnO has emerged as a promising production method due to its advantages of a short process flow, mild reaction conditions, cost-effective catalysts, and the capability to co-produce various products. However, at the current stage, the reaction kinetic equations and optimal conditions for 1,4-butanediol formation via direct hydrogenation of maleic anhydride over Cu-ZnO remain unclear, which hinders the development of this production process.</div><div>In this study, based on the findings of density functional theory, this study investigated the reaction kinetics of direct hydrogenation of maleic anhydride on Cu211 surfaces and at Cu211-ZnO interfaces using activity evaluation experiments and kinetic Monte Carlo simulations. Through activity evaluation experiments of direct hydrogenation of maleic anhydride, this study examined the effects of temperature, pressure, and hydrogen-to-anhydride ratio on product formation over Cu-ZnO catalysts and identified the optimal reaction conditions for 1,4-butanediol production as 200 °C, 2 MPa, and a hydrogen-to-anhydride ratio of 150. Utilizing the kinetic Monte Carlo method, this study calculated the reaction processes for the direct hydrogenation of maleic anhydride to γ-butyrolactone on Cu211 surfaces and to γ-butyrolactone, 1,4-butanediol, and tetrahydrofuran at Cu211-ZnO interfaces. The optimal reaction conditions for the formation of maleic anhydride to γ-butyrolactone, 1,4-butanediol, and tetrahydrofuran were obtained, respectively. Finally, intrinsic reaction kinetic equations for the direct hydrogenation of maleic anhydride to different products were fitted and derived.</div><div>The obtained intrinsic reaction kinetic equations can be applied in the design of actual reactors or process development after considering the influence of diffusion or directly used in studies where diffusion effects are insignificant. This provides a design foundation for the construction of production processes for direct hydrogenation of maleic anhydride to 1,4-butanediol over Cu-ZnO. It is hoped that this study can offer insights and guidance for the understanding of the direct hydrogenation process of maleic anhydride and the development of the biodegradable plastics industry.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114908"},"PeriodicalIF":3.9,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143378628","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":"Visible-light assisted hydrogen evolution via water splitting over micro-fluidized Cu-doped polymeric carbon nitride sheets","authors":"Shalini Sahani ,&nbsp;TaeYoung Kim ,&nbsp;Shakila Parveen Asrafali ,&nbsp;Sung Soo Han","doi":"10.1016/j.mcat.2025.114895","DOIUrl":"10.1016/j.mcat.2025.114895","url":null,"abstract":"<div><div>Hydrogen production via photocatalytic water splitting was investigated by Cu-doped polymeric carbon nitride and Cu-doped substrate under visible light irradiation. The results showed that Cu-doped substrate exhibited higher hydrogen production in the visible range than bare polymeric carbon nitride. Notably, the photocatalytic power of prepared photocatalysts as the hydrogen evolution rate was recorded as ∼1422 μmolg⁻¹ h⁻¹ which is 38 manifolds than bulk polymeric carbon nitride. This is because Cu-doped polymeric carbon nitride-based heterostructure confines the band alignment which harvests solar light in the visible range. Also, the doped Cu on the porous PCN sheet-like structure boosts the charge carrier's separation resulting high H₂ yield. The apparent quantum yield of Cu-doped PCN's hydrogen generation is 5.75 % at 420 nm.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114895"},"PeriodicalIF":3.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143376489","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":"Structure-guided protein engineering of a novel characterized deoxynivalenol-degrading enzyme from Acidobacteriota provokes enhanced catalytic efficiency","authors":"Jiafeng Niu,&nbsp;Bin Ma,&nbsp;Juan Shen,&nbsp;Hao Zhu,&nbsp;Huibing Chi,&nbsp;Zhaoxin Lu,&nbsp;Fengxia Lu,&nbsp;Ping Zhu","doi":"10.1016/j.mcat.2025.114827","DOIUrl":"10.1016/j.mcat.2025.114827","url":null,"abstract":"<div><div>Deoxynivalenol (DON), a typical <em>Fusarium</em> mycotoxin widely distributed in food and feed samples, which poses a global public health risk to humans and animals. Enzymatic detoxification of DON represents a promising approach to control DON contamination. In this work, a novel DON-degrading enzyme (AADH) was characterized from <em>Acidobacteriota</em> with low similarity to other reported DON-degrading enzymes. AADH displayed the highest activity at pH 7.5 and 35℃, and retained &gt;50 % activity after incubation at 40℃ for 3 h AADH exhibited great pH stability in the pH range of 5.5–10.0, retaining approximately 60 % residual activities after incubation at 4℃ for 12 h Sequentially, structure-guided multiple sequence alignment was applied to enhance the catalytic activity of AADH. In this endeavor, the best mutant E49Q showed a 3.78-fold increase in the specific activity and a 4.06-fold increase in catalytic efficiency (<em>k</em>_cat/<em>K</em>_m) compared to those of wild-type AADH. Substrate channel analysis, molecular dynamics (MD) simulations, and electrostatic potential analysis suggested that the enhanced catalytic efficiency of E49Q was attributed to the reshaped substrate channel shapes, the shortened attack distance, and the enhanced electrostatic interactions. Accordingly, AADH was generated with improved catalytic efficiency. These results enriched the DON-degrading enzyme libraries, which is of great significance for solving the problem of DON contamination.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114827"},"PeriodicalIF":3.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143376490","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":"MoS2-modified metal-organic layer Z-scheme heterojunction for photocatalytic removal of organic dyes: Influencing factors and mechanism","authors":"Keren Shi ,&nbsp;Jiayu Luo ,&nbsp;Ziyan Wang ,&nbsp;Yanshu Zhu ,&nbsp;Fuke Wang ,&nbsp;Jingyang Mu ,&nbsp;Huiqin Yao","doi":"10.1016/j.mcat.2025.114906","DOIUrl":"10.1016/j.mcat.2025.114906","url":null,"abstract":"<div><div>In this study, MoS₂-modified nickel-based organic layer MoS₂/Ni-MOLs (MNM) composites were prepared in situ using a two-step hydrothermal method. The photocatalytic performance of the composites was evaluated by photocatalytic removal of the organic pollutant methylene blue (MB). The results showed that the 1:1 ratio of the composites had the best photocatalytic performance. The degradation efficiency reached 96.74 % within 180 min, and the degradation rate constants were 2.22 and 2.36 times higher than those of MoS₂ and Ni-MOLs, respectively. The degradation rate of MNM was increased to 99.47 % by optimizing the initial concentration of MB and pH. The free radical capture tests identified<span><math><mrow><mspace></mspace><msubsup><mrow><mo>•</mo><mrow><mi>O</mi></mrow></mrow><mrow><mn>2</mn></mrow><mo>−</mo></msubsup></mrow></math></span> and h⁺ as the main reactive radicals. The photoelectrochemical properties and the energy band positions of the two monomers revealed the Z-scheme electron conduction mechanism of MNM. In addition, MNM has good stability and reusability. This study provides an effective strategy for the preparation of highly active and stable Z-scheme heterojunction green photocatalysts.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114906"},"PeriodicalIF":3.9,"publicationDate":"2025-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143349299","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":"Highly efficient NiCo alloy catalyst fabricated by MOFs-templated strategy for N-formylation reaction of amines with CO2 and phenylsilane","authors":"Qixuan Li ,&nbsp;Yufei Li ,&nbsp;Rui Fu ,&nbsp;Dawei Gong ,&nbsp;Wenjing Song ,&nbsp;Weizuo Li ,&nbsp;Xin Wang","doi":"10.1016/j.mcat.2025.114896","DOIUrl":"10.1016/j.mcat.2025.114896","url":null,"abstract":"<div><div>N-formylation of amines with carbon dioxide (CO₂) and phenylsilane represents a sustainable and efficient pathway for synthesizing nitrogen-containing compounds, leveraging the growing interest in using CO₂ as a feedstock in organic synthesis. Based on a bimetallic MOFs templating approach, this study synthesized an efficient NiCo alloy catalyst (termed as NiCo/CN-<em>hmta</em>) for the N<em>-</em>formylation reaction of phenylsilane, CO₂, and N-methylbenzene amine. The catalytic performance results indicate that the NiCo/CN-<em>hmta</em> catalyst exhibits high catalytic activity in the N<em>-</em>formylation reaction process. Various characterizations and comparative experiments to explore the reasons for the enhancement in performance of NiCo/CN-<em>hmta</em> for N<em>-</em>formylation reaction. Additionally, there remain many speculative reaction pathways during the N<em>-</em>formylation reaction, and there is significant controversy regarding the order of interactions among phenylsilane, CO₂, and N-methylbenzene amine. Therefore, this study aims to determine the reaction pathway of the MOFs-derived NiCo alloy catalyst in the N<em>-</em>formylation reaction through deuterated experiments, <em>In-situ</em> diffuse reflection infrared Fourier transform spectroscopy (<em>in-situ</em> DRIFTS) and ¹³C NMR tests to capture intermediates during the reaction process. We hope that our research can provide some insights for future applications of alloy catalysts in N<em>-</em>formylation reactions.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114896"},"PeriodicalIF":3.9,"publicationDate":"2025-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143349297","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":"Constructing WO3/Cu2O nanosheet p-n heterojunction photoanode for enhancing PEC water oxidation performance","authors":"Zilong Zhang ,&nbsp;Zikang Wu ,&nbsp;Yan Fang ,&nbsp;Ruyi Wang ,&nbsp;Lingling Wang ,&nbsp;Yihua Chen ,&nbsp;Yong Jia","doi":"10.1016/j.mcat.2025.114893","DOIUrl":"10.1016/j.mcat.2025.114893","url":null,"abstract":"<div><div>Seeking and constructing a suitable p-n heterojunction photoelectrode system is crucial for improving the efficiency of photogenerated electron-hole separation. Herein, the WO₃/Cu₂O heterostructure was successfully constructed on tungsten mesh using a two-step method. The photoelectrochemical (PEC) properties of the photoanodes loaded with different amounts of Cu₂O were investigated by controlling the electrodeposition time. The photocurrent density of the heterojunction with the 60 s electrodeposition time is the highest, reaching 1.47 mA cm⁻² at 1.23 V vs. RHE, which is three times that of WO₃ nanosheets (0.45 mA cm⁻²) grown in situ on tungsten mesh. The improved PEC performance is attributed to the wider light absorption spectrum, enhanced photogenerated carrier transfer efficiency and suppressed electron-hole recombination probability. This study indicates that the WO₃/Cu₂O heterojunction structure grown and constructed in-situ on tungsten mesh has exciting potential for application in efficiency PEC water separation devices. Moreover, it also provides a feasible approach for designing heterostructure systems adapted to complex environments on different substrates to improve PEC efficiency.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114893"},"PeriodicalIF":3.9,"publicationDate":"2025-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143349298","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":"Ammonia synthesis over γ-Al2O3 supported Co-Mo catalysts","authors":"Paweł Adamski ,&nbsp;Michał Zgrzebnicki ,&nbsp;Aleksander Albrecht ,&nbsp;Artur Jurkowski ,&nbsp;Agnieszka Wojciechowska ,&nbsp;Ewa Ekiert ,&nbsp;Krzysztof Sielicki ,&nbsp;Ewa Mijowska ,&nbsp;Glen J. Smales ,&nbsp;Alexey Maximenko ,&nbsp;Dariusz Moszyński","doi":"10.1016/j.mcat.2025.114907","DOIUrl":"10.1016/j.mcat.2025.114907","url":null,"abstract":"<div><div>Novel ammonia synthesis catalysts are sought due to energetic transformation and increasing environmental consciousness. Materials containing cobalt and molybdenum are showing state-of-art activities in ammonia synthesis. The application of γ-alumina support was proposed to enhance the properties of Co-Mo nanoparticles. The wet impregnation of the support was conducted under reduced pressure. The active catalysts were obtained by ammonolysis of precursors. The chemical and phase composition, as well as morphology, porosity, and surface composition of precursors and catalysts, were characterized. The Co-Mo nanoparticles phase composition as well as their size and dispersion were determined using X-ray absorption spectroscopy utilizing synchrotron radiation, electron microscopy, and X-ray scattering. The catalytic activity was tested in the ammonia synthesis process under atmospheric pressure. The activity and stability of the supported catalysts were compared with unsupported cobalt molybdenum nitride Co₃Mo₃N, revealing the superiority of the present approach.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114907"},"PeriodicalIF":3.9,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143348608","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":"Supported Pd-catalyzed regioselective carbonylative indenones synthesis employing oxalic acid as CO source","authors":"Poonam Sharma ,&nbsp;Pushkar Mehara ,&nbsp;Sheetal ,&nbsp;Pralay Das","doi":"10.1016/j.mcat.2025.114891","DOIUrl":"10.1016/j.mcat.2025.114891","url":null,"abstract":"<div><div>Herein, a tandem polystyrene supported palladium (Pd@PS) nanoparticles catalyzed regioselective carbonylative strategy for indenones synthesis has been devised. The present protocol consists of a single-step carbonylative cyclization of <em>o-‑</em>bromo/chloroaryl iodides with internal alkynes using solid and economical oxalic acid as a CO source. The current approach involves some additional benefits such as oxidant and phosphine ligand-free conditions, gram scale applicability, recyclable upto six cycles, and excellent functional group compatibility for diversely substituted indenones in moderate to good yields.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114891"},"PeriodicalIF":3.9,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143348607","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":"Single-atom photocatalysis: A new frontier toward solar energy conversion","authors":"Jia-Qi Chen ,&nbsp;Yue Wu ,&nbsp;Fang-Xing Xiao","doi":"10.1016/j.mcat.2025.114892","DOIUrl":"10.1016/j.mcat.2025.114892","url":null,"abstract":"<div><div>Photocatalysis represents an emerging technology for solving the deteriorating energy crisis and environmental problems by directly harvesting green, renewable, and sustainable solar energy. Due to the maximum atomic utilization efficiency, tunable electronic structures and outstanding catalytic activities, single-atom catalysts (SACs) have emerged as promising candidates for photocatalysis. Although many reviews on single-atom photocatalysis have been reported in the past few years, a comprehensive review devoted to specifically elucidating the generic characteristics of SACs in heterogeneous photocatalysis has so far not yet appeared. In this review, we summarize the latest progress in SACs mediated photocatalysis paired with diverse photocatalytic mechanisms from a fresh insight. Firstly, we elucidate the various synthetic strategies for SACs with a focus on the advantages and disadvantages of each approach. Subsequently, state-of-the-art characterization methods utilized for unleashing the fine structures of single-atom photocatalysts have been concisely overviewed. Furthermore, wide-spread applications of SACs in diverse photocatalytic redox reactions are comprehensively introduced. Finally, the remaining challenges and future opportunities in this booming research field are outlooked for guiding the rational design of robust, stable, and high-performance SACs. Our review could inspire sparkling ideas on how to smartly utilize single atoms for crafting high-efficiency artificial photosystems towards solar energy conversion.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"575 ","pages":"Article 114892"},"PeriodicalIF":3.9,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143209127","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}