ACS Catalysis Pub Date : 2025-04-22DOI: 10.1021/acscatal.5c01543
Sophie C. Schulze, Martin Oestreich
{"title":"Kinetic Resolution of Acyclic 1,3-Diols by Copper-Catalyzed Regioselective Dehydrogenative Si–O-Coupling","authors":"Sophie C. Schulze, Martin Oestreich","doi":"10.1021/acscatal.5c01543","DOIUrl":"https://doi.org/10.1021/acscatal.5c01543","url":null,"abstract":"A nonenzymatic kinetic resolution of acyclic 1,3-diols by regioselective Si–O coupling with a hydrosilane is reported. The in situ-formed Cu–H catalyst with (<i>R</i>,<i>R</i>)-Ph-BPE as the chiral ligand facilitates the enantioselective silylation of one of the two hydroxy groups. The differentiation between both the enantiomers and the regioisomers strongly depends on the choice of the hydrosilane with a bis(4-anisyl)-substituted tertiary hydrosilane giving the best results. A broad range of <i>anti</i>-1,3-diols is resolved with good to high selectivity factors, especially derivatives bearing a cycloprop-1,1-diyl group at the methylene moiety.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"7 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Catalysis Pub Date : 2025-04-22DOI: 10.1021/acscatal.5c00092
Jason Wai-Lok Poon, Yutao Kuang, Nafiseh Moradinik, Chatura Goonesinghe, Salik Hasan Rushdy, Joseph Chang, Takeo Iwase, Maria Ezhova, Savvas G. Hatzikiriakos, Jolene P. Reid, Parisa Mehrkhodavandi
{"title":"Selective Block Copolymerization of Lactide and Methyl Methacrylate with Cationic Indium Catalysts: Exploring the Influence of Noncovalent Ligand Interactions","authors":"Jason Wai-Lok Poon, Yutao Kuang, Nafiseh Moradinik, Chatura Goonesinghe, Salik Hasan Rushdy, Joseph Chang, Takeo Iwase, Maria Ezhova, Savvas G. Hatzikiriakos, Jolene P. Reid, Parisa Mehrkhodavandi","doi":"10.1021/acscatal.5c00092","DOIUrl":"https://doi.org/10.1021/acscatal.5c00092","url":null,"abstract":"Synthesizing a pure, high molecular weight block copolymer of methyl methacrylate (MMA) and lactide (LA) using a one-pot, sequential addition approach is challenging, as these two monomers are generally polymerized via orthogonal mechanisms. In this work, we report the synthesis of PMMA-<i>b</i>-PLA using a cationic indium complex featuring a hemilabile arm. Extensive efforts were made to confirm block copolymer formation, differentiate it from homopolymer blends, and quantify homopolymer impurities. The copolymers were characterized by Size Exclusion Chromatography, Diffusion Ordered NMR Spectroscopy, Differential Scanning Calorimetry, Thermogravimetric Analysis, and fractional precipitation. Block copolymers with tunable molecular weights were synthesized and rheologically characterized, exhibiting enhanced rheo-mechanical properties over PLA and tunable morphologies based on MMA-to-<i>rac</i>-LA ratios. Computational studies revealed that noncovalent interactions between aromatic substituents in the ligand backbone of the cationic indium complex facilitate MMA polymerization, highlighting a unique strategy for tuning polymerization reactivity through ligand design.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"63 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862523","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Catalysis Pub Date : 2025-04-22DOI: 10.1021/acscatal.5c02369
Sandhya Saini, Ranjita S. Das, Anupama Kumar, Suman L. Jain
{"title":"Retraction of “Photocatalytic C–H Carboxylation of 1,3-Dicarbonyl Compounds with Carbon Dioxide Promoted by Nickel(II)-Sensitized α-Fe2O3 Nanoparticles”","authors":"Sandhya Saini, Ranjita S. Das, Anupama Kumar, Suman L. Jain","doi":"10.1021/acscatal.5c02369","DOIUrl":"https://doi.org/10.1021/acscatal.5c02369","url":null,"abstract":"The authors retract this article (DOI: 10.1021/acscatal.2c01483) due to concerns raised that the Nuclear Magnetic Resonance data in Figures 15 and S1–S6, which are the primary means for structural assignment in the organic products of the catalytic reaction at the center of the paper, may not reliably reflect the results of the experiments. As such, this article is being retracted. Co-author Sandhya Saini was unavailable for comments and did not respond/participate in the retraction of this article. The original article was published on April 13, 2022, and was retracted on April 22, 2025. This article has not yet been cited by other publications.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"1 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858095","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Catalysis Pub Date : 2025-04-22DOI: 10.1021/acscatal.5c00273
Yuhan Li, Zhe Huangfu, Youji Li, Xinyuan Song, Youyu Duan, Yi Zhang, Xin Li
{"title":"Asymmetric Chiral Photocatalysts","authors":"Yuhan Li, Zhe Huangfu, Youji Li, Xinyuan Song, Youyu Duan, Yi Zhang, Xin Li","doi":"10.1021/acscatal.5c00273","DOIUrl":"https://doi.org/10.1021/acscatal.5c00273","url":null,"abstract":"Traditional photocatalysts generally have a limitation of weak photoresponsiveness. Although current modification methods can improve light absorption and photoresponsiveness by increasing the surface area and optimizing the bandgap width, the vast majority of visible light has not been effectively utilized. Inorganic chiral photocatalysts can be synthesized using chiral solvents, additives, or templates as inducers. For nonpure phase inorganic chiral photocatalysts, their three-dimensional chiral nematic structure can be used to selectively reflect circularly polarized light, thereby reducing light energy loss and improving the photocatalyst’s light absorption capacity. It is worth noting that the photoactivity of these materials is not dependent on the specific chiral orientation of the structure. For pure phase inorganic chiral photocatalysts, the chirality index and radius would affect the band gap of the photocatalyst. Therefore, by adjusting these parameters, the band structure can be optimized to utilize more visible light, thereby improving the light absorption capacity. Compared to traditional thermal or electrocatalysis, asymmetric photocatalytic reactions offer two distinct advantages: (1) using light as an energy source can reduce dependence on fossil fuels and help achieve a more environmentally friendly and energy-efficient process; (2) photocatalytic reactions, operating through excited-state processes, can achieve transformations that are difficult or impossible to realize through conventional thermal or electrocatalytic methods. Therefore, the development of efficient asymmetric photocatalysts is a core requirement in the field of asymmetric photocatalysis. In contrast, single and dual functional chiral photocatalysts integrate visible light excitation and stereo control in the same catalyst, allowing the induced free radical intermediates to be placed in a chiral configuration. The introduction of chiral structures facilitates the rational design of photocatalytic systems, enabling precise control over the catalytic activity and selectivity. This review delves into the role of chiral ligands in regulating the conformational, electronic, and spatial structures during catalytic reactions, providing important insights for designing catalysts with higher activity and selectivity. Additionally, it summarizes the relationship between chiral ligands and catalytic reaction mechanisms, offering the potential to uncover key steps and reaction kinetics in the catalytic processes. This could provide a more systematic theoretical framework for the precise design of catalysts, thus promoting the widespread industrial application of asymmetric catalytic reactions.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"13 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Catalysis Pub Date : 2025-04-22DOI: 10.1021/acscatal.5c00374
Shicheng Luo, Baorong Xu, Daolin Tan, Weibo Hua, Guocheng Yan, Bo Lin, Guidong Yang
{"title":"Frustrated Lewis-Pair Catalyst Based on Re Single Atoms for Efficient Solar-Driven CO2 Conversion","authors":"Shicheng Luo, Baorong Xu, Daolin Tan, Weibo Hua, Guocheng Yan, Bo Lin, Guidong Yang","doi":"10.1021/acscatal.5c00374","DOIUrl":"https://doi.org/10.1021/acscatal.5c00374","url":null,"abstract":"Owing to the highly efficient activation ability of frustrated Lewis-pair (FLP) sites for small molecules, the development of FLP-based materials is a fascinating route to convert CO<sub>2</sub> to value-added chemicals using solar energy. Herein, rhenium (Re) single atoms are introduced into the frame of graphitic carbon nitride (Re<sub>1</sub>/gCN) to construct unique N···Re<sub>1</sub> FLP sites, where Re single atoms and neighboring N atoms serve as acidic and basic sites, respectively. The N···Re<sub>1</sub> FLP sites can interact with CO<sub>2</sub> molecules to form a Re–O–C-N structure (acid site–basic site–acid site–basic site) via the dramatic d–p orbital interactions, thus inducing an unusual push–push electronic effect to effectively break the C═O bond for CO<sub>2</sub> activation and conversion. As a result, Re<sub>1</sub>/gCN achieves a high photocatalytic CO<sub>2</sub>-to-CO generation rate of 123.4 μmol g<sup>–1</sup> h<sup>–1</sup> (a CO selectivity of 95.6%) without any sacrificial agents, exceeding the majority of state-of-the-art catalysts under similar test conditions.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"91 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Catalysis Pub Date : 2025-04-22DOI: 10.1021/acscatal.5c02503
Sanjiang Pan, Hang Li, Tianyi Wang, Yang Fu, Shenao Wang, Zishuo Xie, Li Wei, Hao Li, Nan Li
{"title":"Addition to “Er-Doping Enhances the Oxygen Evolution Performance of Cobalt Oxide in Acidic Medium”","authors":"Sanjiang Pan, Hang Li, Tianyi Wang, Yang Fu, Shenao Wang, Zishuo Xie, Li Wei, Hao Li, Nan Li","doi":"10.1021/acscatal.5c02503","DOIUrl":"https://doi.org/10.1021/acscatal.5c02503","url":null,"abstract":"In the postpublication review of their 2024 paper, the authors identified three critical methodological improvements: (1) adoption of a more appropriate Shirley background for XPS data fitting; (2) acknowledgment of ongoing academic controversies regarding oxygen vacancy descriptions; (3) implementation of refined analytical methods for quantitative cobalt valence state analysis. While the conclusions of the original manuscript remain unaffected, certain annotations and statements need to be addressed to ensure a more scientifically rigorous XPS analysis. <b>Page 13818, “Results and Discussion”, Sixth Paragraph:</b> The published text reads “Figure 3c depicts the Co<sup>3+</sup>/Co<sup>2+</sup> ratios of 0.97 for 4% Er–Co<sub>3</sub>O<sub>4</sub> and 0.59 for Co<sub>3</sub>O<sub>4</sub>, emphasizing a positive correlation between the Co<sup>3+</sup>/Co<sup>2+</sup> ratio and catalytic OER activity under acidic media.” Here, the discussion on the quantitative analysis of Co valence states should be revised to focus on qualitative analysis. “As shown in Figure 1, the comparison of high-resolution Co 2p XPS spectra between 4% Er–Co<sub>3</sub>O<sub>4</sub>, Co<sub>3</sub>O<sub>4</sub>, and the CoO standard revealed that the satellite peak of Co<sup>2+</sup> at 786 eV exhibited significant suppression in Er–Co<sub>3</sub>O<sub>4</sub>. Meanwhile, the satellite peak of Co<sup>3+</sup> at 790 eV demonstrated a markedly increased proportion in Er–Co<sub>3</sub>O<sub>4</sub>, indicating that Er doping effectively enhances the Co<sup>3+</sup> content in Co<sub>3</sub>O<sub>4</sub>.” <b>Page 13818, “Results and Discussion”, Sixth Paragraph:</b> The published text reads “As Figure 3b shows, the O 1s spectrum contained two distinct oxygen species, including the Co–O bond (labeled as O1) and the oxygen vacancy site (labeled as O2).<sup>41,44</sup> The ratios of O2/O1 in 4% Er–Co<sub>3</sub>O<sub>4</sub> and Co<sub>3</sub>O<sub>4</sub> are 2.63 and 1.69, respectively (Figure 3d).” “Overall, the increase of Co<sup>3+</sup>/Co<sup>2+</sup> and O2/O1 in the sample reconfirmed that Er incorporation increased the lattice defects of Co<sub>3</sub>O<sub>4</sub>, exposing more oxygen vacancies and more high-valence Co ions.” The definition of O2 should be revised to “oxygen defects and hydrates”. Additionally, the O2/O1 ratios require adjustment to 2.70 (A) and 1.56 (B) due to the application of Shirley background subtraction in spectral fitting. “As Figure 2a shows, the O 1s spectrum contained two distinct oxygen species, including the Co–O bond (labeled as O1) and the oxygen defects and hydrates (labeled as O2). The ratios of O2/O1 in 4% Er–Co<sub>3</sub>O<sub>4</sub> and Co<sub>3</sub>O<sub>4</sub> are 2.70 and 1.56, respectively (Figure 2b).” “These findings are consistent with the results obtained from HR-TEM. Overall, the increase of Co<sup>3+</sup>/Co<sup>2+</sup> and O2/O1 in the sample reconfirmed that Er incorporation increased the lattice defects of Co<sub>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"32 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858097","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Remote meta-C–H α-Fluoro-alkenylation of Arenes Using gem-Difluoroalkenes","authors":"Yogesh Bairagi, Sandip Porey, Iti Mahato, Debabrata Maiti","doi":"10.1021/acscatal.5c01455","DOIUrl":"https://doi.org/10.1021/acscatal.5c01455","url":null,"abstract":"Development of efficient and mild methods for the synthesis of arylated α-fluoroalkene motifs has attracted significant interest due to their broad applications in pharmaceuticals and agrochemicals. However, the synthesis of arylated α-fluoroalkenes has been limited to nondirected or directing group (DG)-assisted <i>ortho</i>-C(sp<sup>2</sup>)–H activation. Herein, we report the remote <i>meta</i>-selective α-fluoroalkenylation of arenes. Mechanistic studies have revealed the pivotal functions of a pyrimidine-based DG, palladium catalyst, hexafluoro-isopropanol (HFIP) solvent, and a monoprotected amino acid (MPAA) bidentate ligand in facilitating selective <i>meta</i>-C–H activation, leading to α-fluoroalkenylation with high regioselectivity.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"219 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862529","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Catalysis Pub Date : 2025-04-21DOI: 10.1021/acscatal.5c01859
Eric J. McLaren, Guangshou Feng, Noah H. Watkins, Qiu Wang
{"title":"Copper-Catalyzed Allylic Amination of Alkenes Using O-Acylhydroxylamines: A Direct Entry to Diverse N-Alkyl Allylamines","authors":"Eric J. McLaren, Guangshou Feng, Noah H. Watkins, Qiu Wang","doi":"10.1021/acscatal.5c01859","DOIUrl":"https://doi.org/10.1021/acscatal.5c01859","url":null,"abstract":"We report a copper-catalyzed direct allylic amination of alkenes using readily available <i>O</i>-benzyolhydroxylamines as the alkylamine precursors and internal oxidant. A range of primary and secondary alkylamines can be installed onto diversely substituted alkenes for the rapid construction of <i>N</i>-alkyl allylamines. Mechanistic studies support that the reaction engages an initial electrophilic amination to alkenes with anti-Markovnikov selectivity and subsequently a regioselective oxidative elimination to furnish the double bond transposition. In the electrophilic amination step, the use of strong Brønsted acid is critical for generating the key aminium radical cation (ARC) species.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"63 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Catalysis Pub Date : 2025-04-21DOI: 10.1021/acscatal.5c01779
Tingting Cai, Jie Chen, Linquan Wang, Fangfang Fan, Guo Chen, Shuai Qiu, Na Li, Lehe Mei, Jun Huang
{"title":"Extending the Substrate Scope of an ω-Amine Transaminase from Aspergillus terreus by Reconstructing and Engineering an Ancestral Enzyme","authors":"Tingting Cai, Jie Chen, Linquan Wang, Fangfang Fan, Guo Chen, Shuai Qiu, Na Li, Lehe Mei, Jun Huang","doi":"10.1021/acscatal.5c01779","DOIUrl":"https://doi.org/10.1021/acscatal.5c01779","url":null,"abstract":"Amine transaminases (ATAs) are used for synthesizing chiral amines from prochiral ketones or aldehydes through asymmetric reductive amination. However, there is still an urgent need to develop and evolve more ATAs with good performance, such as high activity, high stability, and wide substrate scope, to adapt to industrial production. Herein, a strategy of <b>A</b>ncestral <b>S</b>equence Reconstruction-<b>C</b>rystal Structure Guided-<b>P</b>ocket Engineering (ASCP) was used to engineer <i>R</i>-selective ω-ATA from <i>Aspergillus terreus</i> (<i>At</i>ATA) for enhancing the thermostability and catalytic performance toward non-natural substrates. Through the ancestral sequence reconstruction (ASR) strategy, an ancestral ω-ATA (Anc101) was acquired, which showed a 10.9 °C enhancement in half-inactivation temperature (<i>T</i><sub>50</sub><sup>10</sup>) and 484-fold improvement in half-life (<i>t</i><sub>1/2</sub>) at 45 °C compared with <i>At</i>ATA. To increase the activities of Anc101 toward non-natural substrates, the substrate binding pocket was modified based on the X-ray crystal structure of Anc101, which we solved at a resolution of 2.3 Å (PDB: 8ZM7). The best mutant Anc1016 (Anc101-H55T-E117S-R128M-V150A-L183F-L188F) showed a 133-fold improvement in catalytic activity toward 3-acetylbiphenyl as compared with Anc101. The conversions using Anc1016 toward all tested substrates were increased by 2–87% compared with Anc101. Mechanism analysis revealed that the “gate ring” covering the cavity entrance of Anc1016 was more flexible than that in Anc101, thereby increasing access of the substrates to the binding pocket. In addition, the total volume of the large and small substrate binding pockets increased. Both of these alterations contribute to the enhanced activities toward non-natural substrates of Anc1016.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"11 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Catalysis Pub Date : 2025-04-21DOI: 10.1021/acscatal.5c01563
Ricardo A. Garcia Carcamo, Jiexin Shi, Ali Estejab, Tianjun Xie, Sanchari Bhattacharjee, Sayani Biswas, Cameron J. Bodenschatz, Xiuting Chen, Manish Maurya, Xiaohong Zhang, Rachel B. Getman
{"title":"A Perspective on Multiscale Modeling of Explicit Solvation-Enabled Simulations of Catalysis at Liquid–Solid Interfaces","authors":"Ricardo A. Garcia Carcamo, Jiexin Shi, Ali Estejab, Tianjun Xie, Sanchari Bhattacharjee, Sayani Biswas, Cameron J. Bodenschatz, Xiuting Chen, Manish Maurya, Xiaohong Zhang, Rachel B. Getman","doi":"10.1021/acscatal.5c01563","DOIUrl":"https://doi.org/10.1021/acscatal.5c01563","url":null,"abstract":"Catalysis at liquid–solid interfaces is profoundly influenced by the interfacial solvent structure, which affects catalytic activity, selectivity, and reaction pathways. This perspective discusses state-of-the-art multiscale modeling methods that integrate quantum mechanics and molecular mechanics approaches to apply explicit solvent molecules to capture these interfacial phenomena. Specifically, the construction of multiscale models, the importance of capturing the interfacial solvent structure, and the computational strategies used to achieve this are explored, and the challenges in balancing chemical accuracy with computational expense are highlighted. Additionally, this perspective addresses the limitations of current methods. Opportunities for integrating machine learning are proposed. By advancing the efficiency and user friendliness of multiscale modeling, it is argued that deeper insights into heterogeneous catalysis in the liquid phase can be provided, which will ultimately contribute to the development of more efficient catalytic processes.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"24 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853340","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}