ACS Publications最新文献

{"title":"The Next Twenty Years of the Journal of Chemical Theory and Computation.","authors":"Qiang Cui, Marco De Vivo, Laura Gagliardi","doi":"10.1021/acs.jctc.4c01067","DOIUrl":"https://doi.org/10.1021/acs.jctc.4c01067","url":null,"abstract":"","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":null,"pages":null},"PeriodicalIF":5.7,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306579","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":"Crystalline Ru-Decorated MOF-Derived Amorphous CoMo-LDH Nanosheet Arrays as Bifunctional Catalysts for Overall Natural Seawater Electrolysis.","authors":"Thuy Tien Nguyen Tran, Thi Anh Le, Nguyen Thi Thu Dinh, Nguyen Duy Hai, Thuy-Kieu Truong, Jianmin Yu, Lishan Peng, Cuong Chi Nguyen, Ngoc Quang Tran","doi":"10.1021/acsami.4c09232","DOIUrl":"https://doi.org/10.1021/acsami.4c09232","url":null,"abstract":"<p><p>The construction of an amorphous/crystalline heterostructure of MOF-derived electrocatalysts offers an intriguing pathway to improve hydrogen production efficiency, but it has received little attention. Here, we report crystalline Ru-decorated MOF-derived amorphous CoMo-LDH nanosheet arrays as highly active and robust bifunctional electrocatalysts for natural seawater electrolysis. Benefiting from the abundant interfaces, the Ru-CoMo-LDH catalyst exhibits excellent activity toward OER under fresh and natural seawater, in particular; it requires only 257 and 406 mV overpotential at 10 and 500 mA cm^-2 in 1 M KOH + Seawater, outperforming the benchmark RuO₂. In addition, this electrocatalyst is an eminently active and stable HER in various electrolytes, emphasizing its outstanding bifunctional capability. Strikingly, in full-cell overall water splitting in natural seawater test, Ru-CoMo-LDH ∥ Pt/C exhibits superior electrochemical behavior (i.e., overpotential of 1.5545 and 1.731 V to obtain the current density of 10 and 200 mA cm^-2, respectively) and high stability. These excellent electrocatalytic activities highlighted the synergistic effects of intimated amorphous/crystalline junctions, which provide a rich population of exposed active sites and enhance electron transport. This, in turn, lowers the adsorption energy barrier of intermediates, leading to improved performance. Our work proves that designing an amorphous/crystalline heterointerface is a promising platform for further enhancing the hydrogen generation efficiency.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306519","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hydrogen Plasma Inhibits Ion Beam Restructuring of GaP.","authors":"John A Scott, James Bishop, Garrett Budnik, Milos Toth","doi":"10.1021/acsami.4c06977","DOIUrl":"https://doi.org/10.1021/acsami.4c06977","url":null,"abstract":"<p><p>Focused ion beam (FIB) techniques are employed widely for nanofabrication and processing of materials and devices. However, ion irradiation often gives rise to severe damage due to atomic displacements that cause defect formation, migration, and clustering within the ion-solid interaction volume. The resulting restructuring degrades the functionality of materials and limits the utility of FIB ablation and nanofabrication techniques. Here we show that such restructuring can be inhibited by performing FIB irradiation in a hydrogen plasma environment via chemical pathways that modify defect binding energies and transport kinetics, as well as material ablation rates. The method is minimally invasive and has the potential to greatly expand the utility of FIB nanofabrication techniques in processing functional materials and devices.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306540","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Engineering Carrier Density and Effective Mass of Plasmonic TiN Films by Tailoring Nitrogen Vacancies.","authors":"Shunda Zhang, Tian-Yu Sun, Zhen Wang, Ruyi Zhang, Yu Lin, Shaozhu Xiao, Guanhua Su, Jiachang Bi, Peiyi Li, Hongliang Zhang, Lingyan Liang, Fang Yang, Qinghua Zhang, Liang-Feng Huang, Yanwei Cao","doi":"10.1021/acs.nanolett.4c03534","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c03534","url":null,"abstract":"<p><p>The introduction of nitrogen vacancies has been shown to be an effective way to tune the plasmonic properties of refractory titanium nitrides. However, its underlying mechanism remains debated due to the lack of high-quality single-crystalline samples and a deep understanding of electronic properties. Here, a series of epitaxial titanium nitride films with varying nitrogen vacancy concentrations (TiN_<i>x</i>) were synthesized. Spectroscopic ellipsometry measurements revealed that the plasmon energy could be tuned from 2.64 eV in stoichiometric TiN to 3.38 eV in substoichiometric TiN_<i>x</i>. Our comprehensive analysis of electrical and plasmonic properties showed that both the increased electronic states around the Fermi level and the decreased carrier effective mass due to the modified electronic band structures are responsible for tuning the plasmonic properties of TiN_<i>x</i>. Our findings offer a deeper understanding of the tunable plasmonic properties in epitaxial TiN_<i>x</i> films and are beneficial for the development of nitride plasmonic devices.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":null,"pages":null},"PeriodicalIF":9.6,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306619","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Using Er/Cd-Codoped Bi₄O₅Br₂ Microspheres to Enhance Antibiotic Degradation under Visible Illumination: A Combined Experimental and DFT Investigation.","authors":"Gaihui Liu, Rong Dai, Huihui Shi, Nan Dong, Bohang Zhang, Shiping Li, Wei Wang, Yang Liu, Tingting Shao, Mengqiong Zhang, Vadivel Subramaniam, Krishnamoorthy Ramachandran, Fuchun Zhang, Xinghui Liu","doi":"10.1021/acs.jpcb.4c04204","DOIUrl":"https://doi.org/10.1021/acs.jpcb.4c04204","url":null,"abstract":"<p><p>High levels of antibiotic accumulation and the difficulty of degradation can have serious consequences for the environment and, therefore, require urgent attention. To solve this problem, a synergistic Er and Cd ion-codoped Bi₄O₅Br₂ photocatalyst was proposed. The degradation rate of sulfamethoxazole (SMX) by Er/Cd-Bi₄O₅Br₂ was eight times higher than that of pure Bi₄O₅Br₂, exceeding that of single Er-doped or Cd-doped Bi₄O₅Br₂, which was attributed to the ability of Er/Cd-Bi₄O₅Br₂ to generate a variety of free radicals. Experimental results and theoretical calculations suggested a possible mechanism for the improved photocatalytic degradation rate. The reduction of the band gap can facilitate the production of electron-hole pairs, which play a significant role in the production of reactive radicals. Furthermore, an optimal stabilized structure of the ErCd-Bi₄O₅Br₂ dopant system was identified based on the formation energy formulas of different ligand configurations. These findings offer promising potential for the degradation of broad-spectrum antibiotics and provide valuable insights for the design and modification of photocatalytic materials.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":null,"pages":null},"PeriodicalIF":2.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306640","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":"Cellular Membrane-Derived Nanovesicles Expressing hCD64 for Targeting Prostate Cancer.","authors":"Sehan Kim, Jeonghyeon Lee, Jaesung Park","doi":"10.1021/acsabm.4c01045","DOIUrl":"https://doi.org/10.1021/acsabm.4c01045","url":null,"abstract":"<p><p>Extracellular vesicles are ideal therapeutic potentiators for various diseases. However, they commonly lack targeting capability and are rapidly cleared by phagocytes. This requires appropriate administration at high doses, which can lead to toxic and adverse reactions. To overcome these limitations, we developed bleb nanovesicles containing human Fcγ receptor I (hCD64), known for their strong affinity to monomeric IgG. In this study, we focused on prostate cancer, which has a specific membrane antigen. We have utilized the hCD64-expressing bleb nanovesicles attaching anti-prostate-specific membrane antigen (PSMA) antibodies and confirmed their targeting ability in PSMA-related cell lines and prostate cancer xenograft models. Our findings underscore the promising potential of nanovesicle Fcγ receptor-IgG as a platform for cancer diagnosis and therapy systems, inspiring further research.</p>","PeriodicalId":2,"journal":{"name":"ACS Applied Bio Materials","volume":null,"pages":null},"PeriodicalIF":4.6,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306515","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Correction to \"Defect Termination in the UiO-66 family of Metal-Organic Frameworks: The Role of Water and Modulator\".","authors":"Kui Tan, Haardik Pandey, Hao Wang, Ever Velasco, Kun-Yu Wang, Hong-Cai Zhou, Jing Li, Timo Thonhauser","doi":"10.1021/jacs.4c12195","DOIUrl":"https://doi.org/10.1021/jacs.4c12195","url":null,"abstract":"","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":null,"pages":null},"PeriodicalIF":14.4,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306593","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":"Improving the Accuracy in the Prediction of Transition-Metal Spin-State Energetics Using a Robust Variation-Based Approach: Density Functional Theory, CASPT2 and MC-PDFT Applied to the Case Study of Tris-Diimine Fe(II) Complexes.","authors":"Gheorghe Paveliuc, Latévi Max Lawson Daku","doi":"10.1021/acs.jpca.4c04148","DOIUrl":"https://doi.org/10.1021/acs.jpca.4c04148","url":null,"abstract":"&lt;p&gt;&lt;p&gt;Designing ligands for transition metal complexes with a specified low-spin, high-spin or spin-crossover behavior is challenging. A major advance was recently made by Phan et al. [&lt;i&gt;J. Am. Chem. Soc.&lt;/i&gt; &lt;b&gt;2017, 139,&lt;/b&gt; 6437-6447] who showed that the spin state of a homoleptic tris-diimine Fe(II) complex can be predicted from the N-N distance in the free diimine. They could thus predict the change in magnetic behavior on passing from the complexes of 2,2'-bipyridine (bpy), 2,2'-biimidazole (bim) and 2,2'-bis-2-imidazoline (bimz) ligands to those obtained with the modified analogs 4,5-diazafluoren-9-one (dafo), 1,1'-(α,α'-&lt;i&gt;o&lt;/i&gt;-xylyl)-2,2'-bisimidazole (xbim) and 2,3,5,6,8,9-hexahydrodiimidazo[1,2-&lt;i&gt;a&lt;/i&gt;:2', 1'-&lt;i&gt;c&lt;/i&gt;]pyrazine (etbimz), respectively. Theoretically, the challenge lies in the accurate determination of the HS-LS zero-point energy difference Δ&lt;i&gt;E&lt;/i&gt;&lt;sub&gt;HL&lt;/sub&gt;&lt;sup&gt;°&lt;/sup&gt;. The issue can be circumvented by using a variation-based approach, wherein Δ&lt;i&gt;E&lt;/i&gt;&lt;sub&gt;HL&lt;/sub&gt;&lt;sup&gt;°&lt;/sup&gt; is not directly evaluated but obtained from the estimate of its variation Δ(Δ&lt;i&gt;E&lt;/i&gt;&lt;sub&gt;HL&lt;/sub&gt;&lt;sup&gt;°&lt;/sup&gt;) in series of related systems, which include one whose Δ&lt;i&gt;E&lt;/i&gt;&lt;sub&gt;HL&lt;/sub&gt;&lt;sup&gt;°&lt;/sup&gt; is accurately known [&lt;i&gt;Phys. Chem. Chem. Phys.&lt;/i&gt; &lt;b&gt;2013, 15,&lt;/b&gt; 3752-3763; &lt;i&gt;J. Phys. Chem. A&lt;/i&gt; &lt;b&gt;2022, 126,&lt;/b&gt; 6221-6235]. In this study, density functional theory (DFT), second-order multireference perturbation theory in its CASPT2 formulation, multiconfigurational pair DFT (MC-PDFT) and its hybrid formulation (HMC-PDFT) have been applied to the determination of Δ(Δ&lt;i&gt;E&lt;/i&gt;&lt;sub&gt;HL&lt;/sub&gt;&lt;sup&gt;°&lt;/sup&gt;) in the pairs of complexes &lt;math&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;msup&gt;&lt;mrow&gt;&lt;mo&gt;[&lt;/mo&gt;&lt;mrow&gt;&lt;mi&gt;F&lt;/mi&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;/mrow&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;mi&gt;p&lt;/mi&gt;&lt;mi&gt;y&lt;/mi&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;]&lt;/mo&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;, &lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;mo&gt;[&lt;/mo&gt;&lt;mrow&gt;&lt;mi&gt;F&lt;/mi&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;/mrow&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mi&gt;d&lt;/mi&gt;&lt;mi&gt;a&lt;/mi&gt;&lt;mi&gt;f&lt;/mi&gt;&lt;mi&gt;o&lt;/mi&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;]&lt;/mo&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/math&gt;, &lt;math&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;msup&gt;&lt;mrow&gt;&lt;mo&gt;[&lt;/mo&gt;&lt;mrow&gt;&lt;mi&gt;F&lt;/mi&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;/mrow&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;mi&gt;m&lt;/mi&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;]&lt;/mo&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;, &lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;mo&gt;[&lt;/mo&gt;&lt;mrow&gt;&lt;mi&gt;F&lt;/mi&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;/mrow&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mi&gt;x&lt;/mi&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;mi&gt;m&lt;/mi&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;]&lt;/mo&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/math&gt; and &lt;math&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;msup&gt;&lt;mrow&gt;&lt;mo&gt;[&lt;/mo&gt;&lt;mrow&gt;&lt;mi&gt;F&lt;/mi&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;/mrow&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;mi&gt;m&lt;/mi&gt;&lt;mi&gt;z&lt;/mi&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;]&lt;/mo&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;, &lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;mo&gt;[&lt;/mo&gt;&lt;mrow&gt;&lt;mi&gt;F&lt;/mi&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;/mrow&gt;&lt;msub&gt;&lt;mrow&gt;&lt;mo&gt;(&lt;/mo&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;mi&gt;t&lt;/mi&gt;&lt;mi&gt;b&lt;/mi&gt;&lt;mi&gt;i&lt;/mi&gt;&lt;mi&gt;m&lt;/mi&gt;&lt;mi&gt;z&lt;/mi&gt;&lt;mo&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/msub&gt;&lt;mo&gt;]&lt;","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":null,"pages":null},"PeriodicalIF":2.7,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306632","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":"Anomalous Reaction Pathways to Methane Production in Photocatalytic Ethanol Oxidation.","authors":"Azam Nasirian, Kihyuk Sung, Hye-Young Jang, Sungju Yu","doi":"10.1021/acsami.4c08729","DOIUrl":"https://doi.org/10.1021/acsami.4c08729","url":null,"abstract":"<p><p>Photocatalytic reduction reactions occasionally utilize sacrificial agents to scavenge photogenerated holes, thus enhancing the kinetics and efficiency of electron harvesting. However, exploring alternative hole-mediated oxidation reactions and their potential impact on photoredox processes is limited. This study investigates the products resulting from the oxidation of ethanol, a commonly used hole scavenger, and the underlying mechanisms involved. We examine a homogeneous eosin Y photoreaction scheme containing a Cu complex coordinated with an N-heterocyclic carbene, a combination often employed in CO₂ conversion. Under visible-light excitation, this photosystem yields methane as an unusual product, alongside acetaldehyde and carbon monoxide. Mechanistic analysis reveals that ethanol undergoes a catalytic cascade involving oxidative processes, C-C bond cleavage, and intermolecular hydrogen atom transfer. Notably, the Lewis-acidic metal center of the Cu complex activates a novel pathway for ethanol oxidation. This work presents the influence of catalyst selection and reaction condition optimization on the emergence of new or unexpected catalytic processes.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306517","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hydrogen Bond Network Shaping Proton Penetration Behavior across Two-Dimensional Nanoporous Materials.","authors":"Zilin Qiao, Zhixuan Ying, Xi Zhou, Kejie Feng, Le Shi","doi":"10.1021/acsami.4c11275","DOIUrl":"https://doi.org/10.1021/acsami.4c11275","url":null,"abstract":"<p><p>In this study, we investigate aqueous proton penetration behavior across four types of two-dimensional (2D) nanoporous materials with similar pore sizes using extensive ReaxFF molecular dynamics simulations. The results reveal significant differences in proton penetration energy barriers among the four kinds of 2D materials, despite their comparable pore sizes. Our analysis indicates that these variations in energy barriers stem from differences in the hydrogen bond (HB) network formed between the 2D nanoporous materials and the aqueous environment. The HB network can be classified into two categories: those formed between the surface of the 2D nanoporous materials and the aqueous environment, and those formed between the edge atoms of the nanopores and the water molecules inside the pores. A strong HB network formed between the surface of the 2D nanoporous materials and the aqueous environment induces an orientational preference of water molecules, resulting in an aggregated water layer with high density. This high-density water region traps protons, making it difficult for them to escape and penetrate the nanopores. On the other hand, a strong HB network formed between the edge atoms of the nanopores and the water molecules inside the pores impedes the rotation and migration of water molecules, further inhibiting proton penetration behavior. To facilitate the proton penetration process, in addition to a sufficiently large pore size, a weak HB network between the 2D nanoporous material and the aqueous environment is necessary.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":null,"pages":null},"PeriodicalIF":8.3,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}