化学•材料最新文献

{"title":"Iron Nanoparticles-Confined Graphene Oxide Membranes Coupled with Sulfite-Based Advanced Reduction Processes for Highly Efficient and Stable Removal of Bromate","authors":"Qian Xiao, Zhe Yang, Wanbin Li, Bo Wei, Hao Guo, Shuili Yu, Qimao Gan, Wenyu Liu, Chuyang Y. Tang","doi":"10.1021/acs.est.4c04392","DOIUrl":"https://doi.org/10.1021/acs.est.4c04392","url":null,"abstract":"Advanced reduction processes (ARPs) are promising for pollutant removal in drinking water treatment. In this study, we demonstrated highly efficient reduction of bromate, a harmful disinfection byproduct, by coupling ARPs with an iron nanoparticles-intercalated graphene oxide (GO@FeNPs) catalytic membrane. In the presence of 1.0 mM sulfite (S(IV)), the GO@FeNPs membrane/S(IV) system achieved nearly complete removal of 80 μg/L bromate in 3 min. The first-order reaction rate constant for bromate removal in this system was 420 ± 42 min^–1, up to 5 orders of magnitude faster than previously reported ARPs. The GO@FeNPs catalytic membrane may offer potential advantages of nanoconfinement and facilitated electron shuttling in addition to the high surface area of the fine FeNPs, leading to the remarkable ARP performance. The GO@FeNPs membrane showed excellent stability, maintaining >97.0% bromate removal over 20 cycles of repeated runs. The membrane can also be applied for fast catalytic reduction of other oxyanions, showing >98.0% removal of nitrate and chlorate. This work may present a viable option for utilizing high-performance reductive catalytic membranes for water decontamination.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325694","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Layer Stacking-Induced Transition to a Kane-Band Semiconductor in Sb2Te3","authors":"Dianlong Zhao, Xinjiang Wang, Xiaoyu Wang, Xueting Wang, Xin He, Yuhao Fu, David J. Singh, Lijun Zhang","doi":"10.1021/acs.jpcc.4c03409","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c03409","url":null,"abstract":"We investigate the electronic properties of phases in the Sb₂Te₃ system based on the alternate AA stacking that was recently experimentally identified in Sb₂Te₃ nanowires. The conventional ABC stacking of these materials is the basis of well-established thermoelectric materials related in part to their complex topological electronic structures. We find topological behavior in AA-stacked Sb₂Te₃, as in the ABC-stacked case, but the carrier pockets are distinctly different from those in the ABC-stacked case. While the electronic structure near the band edges remains three-dimensional with the AA-stacked Sb₂Te₃, it is less so than in the ABC case, particularly for n-type. The band structure shows a Kane band shape in the in-plane direction, with a small band gap and small effective masses. We find an unusual combination of low in-plane effective mass and relatively high optical absorption. This combination is a sought-after feature for infrared detection. AA-stacked Sb₂Te₃ has a quasi-direct band gap (0.14 eV) and ultrasmall hole and electron transport effect masses at low carrier concentrations (e.g., <i>m</i>_e/h(ab)^* ≈ 2 × 10^–2 at 10¹⁷ cm^–3 and 2 × 10^–3 at 10¹⁶ cm^–3). The distinctly different electronic properties of AA-stacked Sb₂Te₃ as compared to the conventional ABC stacking yield different properties that may potentially be exploited in bulk form or in heterostructures. We additionally report results for the hypothetical AA-stacked Bi₂Te₃ sister compound.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325795","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Predicting Anion Redox in Secondary Battery Cathode Materials with a Data-Driven Model","authors":"Nicholas S. Grundish, Brandi Ransom, Austin D. Sendek, Lenson A. Pellouchoud, Yutao Li, Evan J. Reed","doi":"10.1021/acs.jpcc.4c02079","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c02079","url":null,"abstract":"In this study, a new empirical model for predicting the likelihood that a material will exhibit anion redox under cation intercalation is developed with a machine learning approach, and many promising new materials are predicted by applying the model to thousands of candidates. This model is applied to a subset of the Inorganic Crystal Structure Database to determine trends in reported literature materials that can guide design and exploration of new materials that exhibit anion redox to obtain high energy storage capacities without the pitfalls, such as low cyclability, that plague known anion redox materials. Anion redox cathodes improve the energy density of current lithium and sodium secondary batteries owing to their ability to charge compensate mobile cation insertion/extraction through changing the oxidation state of the anion in addition to a transition-metal species. Although the true mechanism through which anion charge compensation occurs has not been fully elucidated, materials that exhibit this phenomenon have recently become the topic of intense interest given their potential to help improve the energy density of secondary batteries beyond current capabilities. Anion close-packed structures and high-valent transition metals are confirmed to be key attributes for enabling anion redox in these materials.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325796","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Theoretical Insights into Electrocatalytic Oxygen Evolution on Se-Doped TiO2","authors":"Niranji Thilini Ekanayake, Nicholas J. Mosey","doi":"10.1021/acs.jpcc.4c04841","DOIUrl":"https://doi.org/10.1021/acs.jpcc.4c04841","url":null,"abstract":"Electrocatalytic water splitting has been identified as a potentially sustainable approach for producing H₂ as an energy carrier. In this study, density functional theory calculations are performed to examine the ability of Se-doped TiO₂ to activate water splitting, with an emphasis on the oxygen evolution reaction (OER). This work complements experimental studies, which have illustrated that doping TiO₂ can enhance the catalytic properties of this material. The results of this work suggest that OER activity on TiO₂ can be enhanced with moderate Se doping levels and indicate that multiple OER reaction pathways may be accessible on Se-doped surfaces. The results may be useful in the context of designing new OER catalysts.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":null,"pages":null},"PeriodicalIF":4.126,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325798","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Operating Mechanism Principles and Advancements for Halide Perovskite-Based Memristors and Neuromorphic Devices","authors":"So-Yeon Kim, Heyi Zhang, Jenifer Rubio-Magnieto","doi":"10.1021/acs.jpclett.4c02170","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02170","url":null,"abstract":"With the advent of the generation of artificial intelligence (AI) based on big data-processing technologies, next-generation memristor and memristive neuromorphic devices have been actively studied with great interest to overcome the von Neumann bottleneck limits. Among various candidates, halide perovskites (HPs) have been in the spotlight as potential candidates for these devices due to their unique switching characteristics with low energy consumption and flexible integration compatibility across various sources for scalability. We outline the characteristics and operating principles of HP-based memristors and their neuromorphic devices. We explain filamentary- and interface-type switching according to the type of conducting pathway occurring inside the active HP layer and the operating mechanisms depending on the species that make up this conducting pathway. We summarize the types and mechanisms of current changes beneficial for neuromorphic device applications and finally organize various suggested analysis tools and physical models to enable experimental determination of switching mechanisms from various perspectives.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325821","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":"Front Cover: A Novel Family of Luminescent Pyrenyl-(N-Heterocyclic Carbene)- Halogenated Coinage Metal Complexes: Synthesis, Crystal Structures, and Optical Properties (Eur. J. Inorg. Chem. 27/2024)","authors":"Yaping Cheng,&nbsp;Geoffrey Gontard,&nbsp;Marie Noelle Rager,&nbsp;Abderrahim Khatyr,&nbsp;Michael Knorr,&nbsp;Hani Amouri","doi":"10.1002/ejic.202482701","DOIUrl":"https://doi.org/10.1002/ejic.202482701","url":null,"abstract":"<p><b>The Front Cover</b> illustrates the synthesis of a family of pyrenyl-(NHC)MCl coinage metal complexes, M=Cu^I, Ag^I and Au^I, (NHC=<i>N</i>-heterocyclic carbene). These compounds are stable and were obtained in high yields. The molecular structures of all complexes were ascertained by X-ray diffraction studies. The use of the chromophoric-(NHC) ligand endows these complexes with emissive properties in the blue region at a similar wavelength to the magical natural blue light created by phytoplankton on the surface of the ocean at nightfall. More information can be found in the Research Article by H. Amouri and co-workers.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":38,"journal":{"name":"European Journal of Inorganic Chemistry","volume":null,"pages":null},"PeriodicalIF":2.2,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ejic.202482701","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142328456","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Correction to “Axially Chiral Trifluoromethylbenzimidazolylbenzoic Acid: A Chiral Derivatizing Agent for α-Chiral Primary Amines and Secondary Alcohols To Determine the Absolute Configuration”","authors":"Michal Kriegelstein, David Profous, Antonín Lyčka, Zdeněk Trávníček, Adam Přibylka, Tereza Volná, Sandra Benická, Petr Cankař","doi":"10.1021/acs.joc.4c02356","DOIUrl":"https://doi.org/10.1021/acs.joc.4c02356","url":null,"abstract":"The correct values for the ¹⁹F NMR chemical shifts and their differences for several compounds appear in the table below. This article has not yet been cited by other publications.","PeriodicalId":57,"journal":{"name":"The Journal of Organic Chemistry","volume":null,"pages":null},"PeriodicalIF":4.354,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325837","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":"Carbonylative Cyclization of 2-Iodofluorobenzenes and 2-Aminophenols with Recyclable Palladium-Complexed Dendrimers on SBA-15: One-Pot Synthesis of Dibenzoxazepinones","authors":"Qian Ye, Gang Xie, Wenyan Hao, Mingzhong Cai","doi":"10.1021/acs.joc.4c01640","DOIUrl":"https://doi.org/10.1021/acs.joc.4c01640","url":null,"abstract":"A novel, efficient, and practical route to dibenzoxazepinones has been developed through a one-pot heterogeneous palladium-catalyzed aminocarbonylation/aromatic nucleophilic substitution (S_NAr) sequence starting from readily available 2-iodofluorobenzenes and 2-aminophenols. The carbonylative cyclization reaction proceeds smoothly in dimethyl sulfoxide (DMSO) at 120 °C with 1,8-diazabicyclo(5.4.0)undec-7-ene (DBU) as the base by using a polyamidoamine (PAMAM)-dendronized SBA-15-supported bidentate phosphine–palladium complex [G(1)-2P-Pd(OAc)₂-SBA-15] as the catalyst under 10 bar of CO, yielding a wide variety of dibenzo[<i>b,e</i>][1,4]oxazepin-11(5<i>H</i>)-one derivatives in good to excellent yields. Moreover, this new heterogenized dendritic palladium catalyst has competitive advantages in that it can be facilely recovered by simple filtration in air and recycled more than eight times without any significant loss of activity. The broad substrate scope, high functional group tolerance, and excellent palladium catalyst recyclability of the reaction make this approach a general, efficient, and economical method for the construction of valuable dibenzoxazepinone derivatives.","PeriodicalId":57,"journal":{"name":"The Journal of Organic Chemistry","volume":null,"pages":null},"PeriodicalIF":4.354,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325833","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":"Proton vs Electron: The Dual Role of Redox-Inactive Metal Ions in Permanganate Oxidation Kinetics","authors":"Mengfan Luo, Heng Zhang, Jianhua Guo, Jia Zhao, Can Feng, Jialong Yin, Chang Xu, Ye Du, Yang Liu, Chuan-Shu He, Bo Lai","doi":"10.1021/acs.est.4c06557","DOIUrl":"https://doi.org/10.1021/acs.est.4c06557","url":null,"abstract":"Redox-inactive metal-ion-driven modulation of the oxidation behavior of high-valent metal–oxo complex has garnered significant interest in biological and chemical synthesis; however, their role in permanganate (Mn(VII)) oxidation for the removal of organic pollutants has been largely neglected. Here, we uncover the impact of six metal ions (i.e., Ca²⁺, Mg²⁺, Ni²⁺, Zn²⁺, Al³⁺, and Sc³⁺) presenting in water environments on Mn(VII) activity. These ions uniformly boost the electron and oxygen transfer capabilities of Mn(VII) while impeding proton transfer, as evidenced by electrochemical tests, thioanisole probe analysis, and the kinetic isotope effect. The observed effects are intricately linked to the Lewis acidity of the metal ions. Further mechanistic insights reveal that Mn(VII) can interact with metal ions without direct reduction. Such interactions modify the electronic configuration of Mn(VII) and create an acidic microenvironment, thus increasing its electrophilicity and the energy barrier for the abstraction of proton from organic substrates. More importantly, the efficacy of Mn(VII) in removing phenolic pollutants is regulated by these ions through changing the driving force for proton and electron transfer, i.e., facilitated at pH &gt; 4.5 and inhibited at lower pH. The contribution of active Mn intermediates is also discussed to reveal the oxidative mechanism of the metal ion/Mn(VII) system. These findings not only facilitate the rational design of Mn(VII) oxidation conditions in the presence of metal ions for water decontamination but also offer an alternative paradigm for enhancing electrophilic oxidation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Strategies To Achieve Long-Term Stability in Lead Halide Perovskite Nanocrystals and Its Optoelectronic Applications","authors":"Shovon Chatterjee, Subarna Biswas, Smruti Sourav, Jyotisman Rath, Syed Akhil, Nimai Mishra","doi":"10.1021/acs.jpclett.4c02240","DOIUrl":"https://doi.org/10.1021/acs.jpclett.4c02240","url":null,"abstract":"The lead halide perovskite (LHP) nanocrystals (NCs) research area is flourishing due to their exceptional properties and great potential for a wide range of applications in optoelectronics and photovoltaics. Yet, despite the momentum in the field, perovskite devices are not yet ready for commercialization due to degradation caused by intrinsic phase transitions and external factors such as moisture, temperature, and ultraviolet (UV) light. To attain long-term stability, we analyze the origin of instabilities and describe different strategies such as surface modification, encapsulation, and doping for long-term viability. We also assess how these stabilizing strategies have been utilized to obtain optoelectronic devices with long-term stability. This Mini-Review also outlines the future direction of each strategy for producing highly efficient and ultrastable LHP NCs for sustainable applications.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":6.475,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325791","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}