Jarod C. Kelly,Amgad Elgowainy,Ram Vijayagopal,Matteo Muratori,Ian Sutherland,Hoseinali Borhan,Hyung Chul Kim,Marcus Alexander
This study presents a cradle-to-grave lifecycle analysis of energy use and greenhouse gas (GHG) emissions for U.S. medium- and heavy-duty vehicles across current (2021) and future (2035) technologies using the Greenhouse gas, Regulated Emissions, and Energy use in Technologies (GREET) model with industry-vetted assumptions. Results vary across vehicle classes but point to common trends: today, battery electric vehicles (BEVs) offer significant (10–60%) GHG emissions reduction compared to diesel internal combustion engine vehicles and are the lowest emissions option per ton-mile of cargo movement, followed by hydrogen fuel cell electric vehicles (FCEVs) (5–50% emissions reduction). Emissions savings depend largely on the duty cycle and fuel economy of the vehicle type. Future vehicle technology advancements result in comparable emission reductions associated with BEVs and hydrogen FCEVs. Weight-limited BEV trucks see less per-ton-mile emissions reduction due to the impact of battery weight on increased vehicle weight and reduced payload capacity. By 2035, improvements in vehicle efficiency can reduce emissions across all powertrains. However, very low levels of emissions require switching vehicles’ use-phase fuel/energy to low-carbon fuels and electricity. Renewable diesel, e-fuels, hydrogen produced from natural gas with carbon capture and storage or renewables, and use of low-carbon electricity can all achieve over 70% reduction in GHG emissions from the current day diesel-based internal combustion engine vehicle.
{"title":"Cradle-to-Grave Lifecycle Analysis of U.S. Medium- and Heavy-Duty Vehicle-Fuel Pathways: A Greenhouse Gas Emissions Assessment of Current (2021) and Future (2035) Technologies","authors":"Jarod C. Kelly,Amgad Elgowainy,Ram Vijayagopal,Matteo Muratori,Ian Sutherland,Hoseinali Borhan,Hyung Chul Kim,Marcus Alexander","doi":"10.1021/acs.est.5c10480","DOIUrl":"https://doi.org/10.1021/acs.est.5c10480","url":null,"abstract":"This study presents a cradle-to-grave lifecycle analysis of energy use and greenhouse gas (GHG) emissions for U.S. medium- and heavy-duty vehicles across current (2021) and future (2035) technologies using the Greenhouse gas, Regulated Emissions, and Energy use in Technologies (GREET) model with industry-vetted assumptions. Results vary across vehicle classes but point to common trends: today, battery electric vehicles (BEVs) offer significant (10–60%) GHG emissions reduction compared to diesel internal combustion engine vehicles and are the lowest emissions option per ton-mile of cargo movement, followed by hydrogen fuel cell electric vehicles (FCEVs) (5–50% emissions reduction). Emissions savings depend largely on the duty cycle and fuel economy of the vehicle type. Future vehicle technology advancements result in comparable emission reductions associated with BEVs and hydrogen FCEVs. Weight-limited BEV trucks see less per-ton-mile emissions reduction due to the impact of battery weight on increased vehicle weight and reduced payload capacity. By 2035, improvements in vehicle efficiency can reduce emissions across all powertrains. However, very low levels of emissions require switching vehicles’ use-phase fuel/energy to low-carbon fuels and electricity. Renewable diesel, e-fuels, hydrogen produced from natural gas with carbon capture and storage or renewables, and use of low-carbon electricity can all achieve over 70% reduction in GHG emissions from the current day diesel-based internal combustion engine vehicle.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"33 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138893","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}
Tao Zhang,Henglin Zhang,Tianhui Zhao,Shiming Song,Jiye Zhang,Luhan Yang,Fengchang Wu
Neonicotinoid insecticides (NEOs) are globally prevalent environmental contaminants. However, their biological half-lives in humans remain poorly characterized. This study employed a controlled mouse pharmacokinetic experiment with human biomonitoring data to elucidate key parameters for selected NEOs. Human biomonitoring provided renal clearance (CLrenal), while controlled mice experiment provided the volume of distribution (Vd); these were combined to estimate the biological half-life. Analysis of 172 paired human urine and blood samples revealed that CLrenal varied substantially among parent NEOs (median: 9.04 to 158 mL/day/kg) and exhibited a distinct structure-dependency. The CLrenal of fused, bicyclic NEOs (i.e., imidacloprid (IMI), thiacloprid (THD), and thiamethoxam (THM)) was governed by water solubility, while that of their nonfused, monocyclic systems (i.e., acetamiprid (ACE), clothianidin (CLO), and dinotefuran (DIN)) was determined by lipophilicity. A one-compartment log–linear regression analysis of intravenous mice data provided robust estimates of Vd, which ranged from 306 to 700 mL/kg body weight for ACE, IMI, and DIN. By combining Vd with human CLrenal, the extrapolated median biological half-life for ACE, IMI, and DIN were 15.5, 24.8, and 53.7 days, respectively, indicating significant potential for bioaccumulation in humans. Uncertainty analysis and sensitivity analyses confirmed the robustness of these prolonged estimates, yielding 95% confidence intervals of 5.53 (ACE) to 157 (DIN) days, with even the most conservative scenario giving a range of 5.17 (ACE) to 17.9 (DIN) days. The prolonged half-life of NEOs indicates a significant potential for bioaccumulation in humans upon continuous exposure, which warrants further investigation regarding its implications for human health risk assessment.
{"title":"Combining Biomonitoring Data and a Pharmacokinetic Model to Estimate the Extended Half-Life of Neonicotinoid Insecticides in Humans","authors":"Tao Zhang,Henglin Zhang,Tianhui Zhao,Shiming Song,Jiye Zhang,Luhan Yang,Fengchang Wu","doi":"10.1021/acs.est.5c18046","DOIUrl":"https://doi.org/10.1021/acs.est.5c18046","url":null,"abstract":"Neonicotinoid insecticides (NEOs) are globally prevalent environmental contaminants. However, their biological half-lives in humans remain poorly characterized. This study employed a controlled mouse pharmacokinetic experiment with human biomonitoring data to elucidate key parameters for selected NEOs. Human biomonitoring provided renal clearance (CLrenal), while controlled mice experiment provided the volume of distribution (Vd); these were combined to estimate the biological half-life. Analysis of 172 paired human urine and blood samples revealed that CLrenal varied substantially among parent NEOs (median: 9.04 to 158 mL/day/kg) and exhibited a distinct structure-dependency. The CLrenal of fused, bicyclic NEOs (i.e., imidacloprid (IMI), thiacloprid (THD), and thiamethoxam (THM)) was governed by water solubility, while that of their nonfused, monocyclic systems (i.e., acetamiprid (ACE), clothianidin (CLO), and dinotefuran (DIN)) was determined by lipophilicity. A one-compartment log–linear regression analysis of intravenous mice data provided robust estimates of Vd, which ranged from 306 to 700 mL/kg body weight for ACE, IMI, and DIN. By combining Vd with human CLrenal, the extrapolated median biological half-life for ACE, IMI, and DIN were 15.5, 24.8, and 53.7 days, respectively, indicating significant potential for bioaccumulation in humans. Uncertainty analysis and sensitivity analyses confirmed the robustness of these prolonged estimates, yielding 95% confidence intervals of 5.53 (ACE) to 157 (DIN) days, with even the most conservative scenario giving a range of 5.17 (ACE) to 17.9 (DIN) days. The prolonged half-life of NEOs indicates a significant potential for bioaccumulation in humans upon continuous exposure, which warrants further investigation regarding its implications for human health risk assessment.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"90 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138929","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}
A green and mild palladium-catalyzed solvent-free α-arylation reaction of ketones was disclosed for the first time. Using the robust N-heterocyclic carbene–palladium complex (SIPr)Ph2Pd(cin)Cl, (hetero)aryl chlorides and ketones were able to generate monoarylation products in excellent yields under solvent-free conditions, with a total of 41 examples. Furthermore, the protocol has been demonstrated to be suitable for multigram-scale preparation with a high yield.
{"title":"Solvent-Free α-Arylation Reaction of Ketones with (Hetero)aryl Chlorides by N-Heterocyclic Carbene–Palladium Complex (SIPr)Ph2Pd(cin)Cl","authors":"Jia-Sheng Ouyang,Xiaoling Wang,Huizhen Jiang,Ruiyong Luo,Liqun Hu,Yaqi Zhang,Liqin Qiu","doi":"10.1021/acs.joc.5c02510","DOIUrl":"https://doi.org/10.1021/acs.joc.5c02510","url":null,"abstract":"A green and mild palladium-catalyzed solvent-free α-arylation reaction of ketones was disclosed for the first time. Using the robust N-heterocyclic carbene–palladium complex (SIPr)Ph2Pd(cin)Cl, (hetero)aryl chlorides and ketones were able to generate monoarylation products in excellent yields under solvent-free conditions, with a total of 41 examples. Furthermore, the protocol has been demonstrated to be suitable for multigram-scale preparation with a high yield.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"83 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139055","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}
Pub Date : 2026-02-09DOI: 10.1021/acs.jpclett.5c03884
Elena V. Bodiago, Iuliia A. Melchakova, Sergey V. Makarov, Dmitry S. Gets
In perovskite laser development, it is important to focus on two different regimes of electrical losses: low-power excitation (carrier density lower than 1018 cm–3), when nonradiative processes via trap states can dominate, and high-power excitation (carrier density is 1018–1021 cm–3), when Auger recombination prevails. Therefore, passivating the defects that affect radiative recombination is crucial for lowering the lasing threshold and achieving a high optical gain before the Auger onset. Here, we report a combined laser-induced photothermochemical method for the passivation of surface defects by potassium doping in perovskite. This approach yields improved morphology, an optical gain of up to 2600 cm–1, and operational stability under ambient conditions of 35 million laser shots, with only 15% degradation at excitation densities three times above the threshold. The remarkable performance of this laser-induced process will facilitate the development of modern optical applications, including lasing, morphology-controlled photoluminescence yield, and optical information encryption.
{"title":"Laser-Induced Enhancement of Optical Gain and Stability in Potassium-Doped CsPbBr3 Perovskite Films","authors":"Elena V. Bodiago, Iuliia A. Melchakova, Sergey V. Makarov, Dmitry S. Gets","doi":"10.1021/acs.jpclett.5c03884","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c03884","url":null,"abstract":"In perovskite laser development, it is important to focus on two different regimes of electrical losses: low-power excitation (carrier density lower than 10<sup>18</sup> cm<sup>–3</sup>), when nonradiative processes via trap states can dominate, and high-power excitation (carrier density is 10<sup>18</sup>–10<sup>21</sup> cm<sup>–3</sup>), when Auger recombination prevails. Therefore, passivating the defects that affect radiative recombination is crucial for lowering the lasing threshold and achieving a high optical gain before the Auger onset. Here, we report a combined laser-induced photothermochemical method for the passivation of surface defects by potassium doping in perovskite. This approach yields improved morphology, an optical gain of up to 2600 cm<sup>–1</sup>, and operational stability under ambient conditions of 35 million laser shots, with only 15% degradation at excitation densities three times above the threshold. The remarkable performance of this laser-induced process will facilitate the development of modern optical applications, including lasing, morphology-controlled photoluminescence yield, and optical information encryption.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"6 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146449","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}
Metal–organic frameworks (MOFs), with their distinctive porous structures and tunable chemical properties, have shown immense promise in the separation and storage of gases. Currently, the accurate simulation of their adsorptive properties remains challenging, especially for systems where the molecules fit very tightly into the pores. Traditional simulation methods often approximate the frameworks as rigid and do not account for the framework flexibility seen in materials such as NbOFFIVE-1-Ni. First-principles molecular dynamics (FPMD) simulations offer the desired accuracy in modeling this flexibility but are limited by their extensive computational demands, rendering them impractical for long simulations. Conversely, classical force field-based simulations offer computational efficiency but lack the necessary accuracy. To break this accuracy-efficiency trade-off, we have developed machine learning interatomic potentials trained on energies and forces from FPMD to model the framework flexibility of NbOFFIVE-1-Ni in the presence of water over nanosecond time scales. Furthermore, by integrating MLIP-driven molecular dynamics (MLIP-MD) with grand canonical Monte Carlo (GCMC) simulations, we further incorporated framework flexibility into adsorption predictions, yielding water adsorption isotherms that better align with experimental data compared to those of conventional GCMC simulations. These advances offer new opportunities for the design and optimization of MOFs in gas storage and separation applications.
{"title":"Machine Learning Interatomic Potentials for Modeling Framework Flexibility and Water Uptake in NbOFFIVE-1-Ni Metal–Organic Framework","authors":"Xijun Wang, Xiaoliang Wang, Xiaoyi Zhang, Zhao Li, Jiayang Liu, Faramarz Joodaki, Kaihang Shi, Filip Formalik, Omar K. Farha, Daniela Kohen, Randall Q. Snurr","doi":"10.1021/acs.jpcc.6c00023","DOIUrl":"https://doi.org/10.1021/acs.jpcc.6c00023","url":null,"abstract":"Metal–organic frameworks (MOFs), with their distinctive porous structures and tunable chemical properties, have shown immense promise in the separation and storage of gases. Currently, the accurate simulation of their adsorptive properties remains challenging, especially for systems where the molecules fit very tightly into the pores. Traditional simulation methods often approximate the frameworks as rigid and do not account for the framework flexibility seen in materials such as NbOFFIVE-1-Ni. First-principles molecular dynamics (FPMD) simulations offer the desired accuracy in modeling this flexibility but are limited by their extensive computational demands, rendering them impractical for long simulations. Conversely, classical force field-based simulations offer computational efficiency but lack the necessary accuracy. To break this accuracy-efficiency trade-off, we have developed machine learning interatomic potentials trained on energies and forces from FPMD to model the framework flexibility of NbOFFIVE-1-Ni in the presence of water over nanosecond time scales. Furthermore, by integrating MLIP-driven molecular dynamics (MLIP-MD) with grand canonical Monte Carlo (GCMC) simulations, we further incorporated framework flexibility into adsorption predictions, yielding water adsorption isotherms that better align with experimental data compared to those of conventional GCMC simulations. These advances offer new opportunities for the design and optimization of MOFs in gas storage and separation applications.","PeriodicalId":61,"journal":{"name":"The Journal of Physical Chemistry C","volume":"13 1","pages":""},"PeriodicalIF":4.126,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146485","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}
Bin Lu,Yueming Lucy Qiu,Zhaohua Wang,Bo Wang,Kaifang Luo,Pengfei Liu,Yingdan Mei,Bin Zhang,Jingyun Li
Hydrogen is expected to play a key role in the sustainable decarbonization of energy systems. While hydrogen may provide global public good for reducing carbon emissions, it is important to quantify its potential impact on local communities for ensuring equitable and socially accepted energy transitions. This study quantifies the effects of hydrogen infrastructure on nearby communities by using a high-resolution panel of residential property transactions in California from 2012 to 2021. The analysis incorporates three types of hydrogen infrastructure: hydrogen refueling stations (HRSs), hydrogen production facilities (HPFs), and hydrogen corridor pipelines (HCPs). Our findings show that residential properties within a 2.2 km radius of an HRS experience an average devaluation of 2.74%–3.45% (or US$19,413–$24,444). Following a major hydrogen explosion, this depreciation intensifies to 4.41%–5.28%. HPFs also exert significant negative externalities, with property values declining by 4.52%–5.64% within a 4 km radius. Heterogeneity analyses reveal that minority communities, particularly those with low shares of White residents and high proportions of Black and Hispanic populations, experienced disproportionately greater devaluation. Our empirical evidence of the local impact can help policymakers better systematically promote the larger scale of hydrogen energy deployment while minimizing the potential negative impacts on local communities.
{"title":"Quantifying the Local Impact of Hydrogen Infrastructure: Evidence from Changes in Property Values in California","authors":"Bin Lu,Yueming Lucy Qiu,Zhaohua Wang,Bo Wang,Kaifang Luo,Pengfei Liu,Yingdan Mei,Bin Zhang,Jingyun Li","doi":"10.1021/acs.est.5c08792","DOIUrl":"https://doi.org/10.1021/acs.est.5c08792","url":null,"abstract":"Hydrogen is expected to play a key role in the sustainable decarbonization of energy systems. While hydrogen may provide global public good for reducing carbon emissions, it is important to quantify its potential impact on local communities for ensuring equitable and socially accepted energy transitions. This study quantifies the effects of hydrogen infrastructure on nearby communities by using a high-resolution panel of residential property transactions in California from 2012 to 2021. The analysis incorporates three types of hydrogen infrastructure: hydrogen refueling stations (HRSs), hydrogen production facilities (HPFs), and hydrogen corridor pipelines (HCPs). Our findings show that residential properties within a 2.2 km radius of an HRS experience an average devaluation of 2.74%–3.45% (or US$19,413–$24,444). Following a major hydrogen explosion, this depreciation intensifies to 4.41%–5.28%. HPFs also exert significant negative externalities, with property values declining by 4.52%–5.64% within a 4 km radius. Heterogeneity analyses reveal that minority communities, particularly those with low shares of White residents and high proportions of Black and Hispanic populations, experienced disproportionately greater devaluation. Our empirical evidence of the local impact can help policymakers better systematically promote the larger scale of hydrogen energy deployment while minimizing the potential negative impacts on local communities.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"29 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138895","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}
Utilizing an LC/MS-MS-based feature-based molecular networking (FBMN) strategy, six undescribed PPAPs (1–6) characterized by an acetyl substituent at the C-1 position of their phloroglucinol scaffold, were efficiently isolated from the roots of Harrisonia perforata. Notably, compund 1 displays an unconventional 5/5/6/5 ring architecture, while compounds 5 and 6 represent the first case incorporating a benzofuran core and a geranyl-derived cyclohexanol unit. Their structures were unequivocally elucidated through comprehensive spectroscopic data analysis, TDDFT-ECD calculations, and X-ray crystallographic studies. Interestingly, compound 3 at 20 μM exhibited negligible cytotoxicity but significantly potentiated the activity of paclitaxel against HCT-15 cells by 42.8-fold. Mechanistic studies further demonstrated that compound 3 did not significantly alter the expression levels of ATP-binding cassette (ABC) transporters, but potently inhibited the transport function of both ABCB1 and ABCG2. Molecular docking reveals that compound 3 stably binds to the central substrate-binding cavities of ABCB1 and ABCG2, with its binding primarily stabilized by hydrogen bonds and hydrophobic interactions.
利用基于LC/ ms - ms的特征分子网络（FBMN）策略，从穿孔果harrison根部有效分离出6个未描述的PPAPs(1-6)，其间苯三酚支架的C-1位置具有乙酰取代基。值得注意的是，化合物1具有非常规的5/5/6/5环状结构，而化合物5和6是首次包含苯并呋喃核心和香叶基衍生环己醇单元的情况。通过全面的光谱数据分析、TDDFT-ECD计算和x射线晶体学研究，明确了它们的结构。有趣的是，化合物3在20 μM下的细胞毒性可以忽略不计，但紫杉醇对HCT-15细胞的活性显著增强了42.8倍。机制研究进一步表明，化合物3没有显著改变atp结合盒（ABC）转运蛋白的表达水平，但能有效抑制ABCB1和ABCG2的转运功能。分子对接发现，化合物3与ABCB1和ABCG2的中心底物结合空腔稳定结合，其结合主要通过氢键和疏水相互作用来稳定。
{"title":"Harperoids A–F, Complex Polyprenylated Acylphloroglucinols from Harrisonia perforata that Reverse Multidrug Resistance by Targeting ABC Transporter Function","authors":"Pei-Pei An,Ying Li,Jin-Hai Yu,Bin Zhou,Jian-Min Yue","doi":"10.1021/acs.joc.5c03053","DOIUrl":"https://doi.org/10.1021/acs.joc.5c03053","url":null,"abstract":"Utilizing an LC/MS-MS-based feature-based molecular networking (FBMN) strategy, six undescribed PPAPs (1–6) characterized by an acetyl substituent at the C-1 position of their phloroglucinol scaffold, were efficiently isolated from the roots of Harrisonia perforata. Notably, compund 1 displays an unconventional 5/5/6/5 ring architecture, while compounds 5 and 6 represent the first case incorporating a benzofuran core and a geranyl-derived cyclohexanol unit. Their structures were unequivocally elucidated through comprehensive spectroscopic data analysis, TDDFT-ECD calculations, and X-ray crystallographic studies. Interestingly, compound 3 at 20 μM exhibited negligible cytotoxicity but significantly potentiated the activity of paclitaxel against HCT-15 cells by 42.8-fold. Mechanistic studies further demonstrated that compound 3 did not significantly alter the expression levels of ATP-binding cassette (ABC) transporters, but potently inhibited the transport function of both ABCB1 and ABCG2. Molecular docking reveals that compound 3 stably binds to the central substrate-binding cavities of ABCB1 and ABCG2, with its binding primarily stabilized by hydrogen bonds and hydrophobic interactions.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"90 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139057","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}
Graphene has emerged as a promising candidate for adsorption and separation applications due to its exceptional properties. In this study, the diffusion properties and local structure of the CO2-NO flue gas, CH4, and H2O mixtures in the free state and those confined within graphene layers were investigated via molecular dynamics simulation. Additionally, density functional theory calculation was performed to determine the adsorption energies of these four components at different adsorption sites on graphene. The results showed that the graphene structure significantly altered the diffusion coefficients of the four substances, with the order becoming CH4 > NO > CO2 ≫ H2O. By contrast, in the absence of graphene at low temperatures, the diffusion coefficient order was H2O > CO2 > NO > CH4. Simultaneously, the temperature and pressure exerted pronounced regulatory effects on CH4, CO2, and NO. Analysis of the relative diffusion coefficients of CH4 and NO revealed that the optimal conditions for the adsorption and separation of this mixture with bilayer graphene structures were 1-10 MPa and 275 K.
石墨烯由于其特殊的性能，已成为吸附和分离应用的有前途的候选者。在本研究中，通过分子动力学模拟研究了CO2-NO烟气、CH4和H2O混合物在自由状态和石墨烯层内的扩散特性和局部结构。此外，通过密度泛函理论计算，确定了这四种组分在石墨烯上不同吸附位点的吸附能。结果表明，石墨烯结构显著改变了四种物质的扩散系数，其顺序为CH4 > NO > CO2比H2O。相反，在低温条件下，没有石墨烯时，扩散系数的顺序为H2O > CO2 > NO > CH4。同时，温度和压力对CH4、CO2和NO具有显著的调节作用。对CH4和NO的相对扩散系数分析表明，该混合物与双层石墨烯结构的最佳吸附和分离条件为1-10 MPa和275 K。
{"title":"Transformation of Diffusion and Local Structure of CH<sub>4</sub>, CO<sub>2</sub>, NO, and H<sub>2</sub>O Mixtures into Bilayers Graphene: A Molecular Dynamics and Density Functional Theory Study.","authors":"Ruoting Xu, Chundi Liao, Wei Gao, Yaping Tao, Chunjin Li, Guancun Kong, Guoxian Li, Huajie Feng","doi":"10.1021/acs.jpcb.5c06901","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c06901","url":null,"abstract":"<p><p>Graphene has emerged as a promising candidate for adsorption and separation applications due to its exceptional properties. In this study, the diffusion properties and local structure of the CO<sub>2</sub>-NO flue gas, CH<sub>4</sub>, and H<sub>2</sub>O mixtures in the free state and those confined within graphene layers were investigated via molecular dynamics simulation. Additionally, density functional theory calculation was performed to determine the adsorption energies of these four components at different adsorption sites on graphene. The results showed that the graphene structure significantly altered the diffusion coefficients of the four substances, with the order becoming CH<sub>4</sub> > NO > CO<sub>2</sub> ≫ H<sub>2</sub>O. By contrast, in the absence of graphene at low temperatures, the diffusion coefficient order was H<sub>2</sub>O > CO<sub>2</sub> > NO > CH<sub>4</sub>. Simultaneously, the temperature and pressure exerted pronounced regulatory effects on CH<sub>4</sub>, CO<sub>2</sub>, and NO. Analysis of the relative diffusion coefficients of CH<sub>4</sub> and NO revealed that the optimal conditions for the adsorption and separation of this mixture with bilayer graphene structures were 1-10 MPa and 275 K.</p>","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.9,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146140339","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}
Poonam Saini, Krishna Kumar M. S., Pritam Mukhopadhyay
A dual route involving oxidants under heterogeneous conditions (PbO2) or basic biphasic conditions, i.e., K3[Fe(CN)6]/KOH to C–N bond-forming pyrrole-fused PDIs is developed. These routes avoid the stringent conditions required for coupling reactions or other multistep processes used to date, to realize these functional PDIs. Importantly, both routes proceed at room temperature with short reaction times. In addition, the Br atom is tolerated during cyclization. These multistate redox-active pyrrole-fused PDIs generate blue-colored radical anions and red dianions chemically/electrochemically.
{"title":"Straightforward Dual Oxidative Cyclization Routes Enable Easy Access to Multifunctional Pyrrole-Fused Perylene Diimides","authors":"Poonam Saini, Krishna Kumar M. S., Pritam Mukhopadhyay","doi":"10.1021/acs.joc.5c02492","DOIUrl":"https://doi.org/10.1021/acs.joc.5c02492","url":null,"abstract":"A dual route involving oxidants under heterogeneous conditions (PbO<sub>2</sub>) or basic biphasic conditions, i.e., K<sub>3</sub>[Fe(CN)<sub>6</sub>]/KOH to C–N bond-forming pyrrole-fused PDIs is developed. These routes avoid the stringent conditions required for coupling reactions or other multistep processes used to date, to realize these functional PDIs. Importantly, both routes proceed at room temperature with short reaction times. In addition, the Br atom is tolerated during cyclization. These multistate redox-active pyrrole-fused PDIs generate blue-colored radical anions and red dianions chemically/electrochemically.","PeriodicalId":57,"journal":{"name":"Journal of Organic Chemistry","volume":"3 1","pages":""},"PeriodicalIF":4.354,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146336","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}
Pub Date : 2026-02-09DOI: 10.1021/acs.jpclett.5c04038
Zhenke Zhong, Qiming Lei, Jianhui Chang, Na Li, Jianxiong Xu, Lijian Xu, Hengyue Li, Junliang Yang
Interfacial defects in triple-cation perovskite films limit device efficiency and stability, and passivation strategies often face a critical trade-off between defect coverage and charge transport. We propose a uniform interfacial passivation approach using 2-(1-cyclohexenyl)ethylammonium iodide (CHEAI) with a mixed solvent system of chlorobenzene (CB) and isopropanol (IPA). Based on CHEAI passivation, the CB/IPA mixed solvent system manipulates solvent polarity gradients to induce molecular self-assembly, constructing a uniform two-dimensional(2D) perovskite interfacial layer that enables effective defect passivation and rapid charge transport, thereby addressing this trade-off. This strategy achieves a power conversion efficiency (PCE) of 25.72% and a fill factor (FF) of 86.27%, the highest reported values for conventional two-step method-based triple-cation perovskite solar cells (PSCs). Moreover, it demonstrates effectiveness in systems with different passivating agents. This study provides a straightforward and effective approach to improving the efficiency and stability of PSCs.
{"title":"Achieving Efficient Triple-Cation Perovskite Solar Cells with Fill Factor Exceeding 86% via a Uniform Interface Passivation Strategy","authors":"Zhenke Zhong, Qiming Lei, Jianhui Chang, Na Li, Jianxiong Xu, Lijian Xu, Hengyue Li, Junliang Yang","doi":"10.1021/acs.jpclett.5c04038","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c04038","url":null,"abstract":"Interfacial defects in triple-cation perovskite films limit device efficiency and stability, and passivation strategies often face a critical trade-off between defect coverage and charge transport. We propose a uniform interfacial passivation approach using 2-(1-cyclohexenyl)ethylammonium iodide (CHEAI) with a mixed solvent system of chlorobenzene (CB) and isopropanol (IPA). Based on CHEAI passivation, the CB/IPA mixed solvent system manipulates solvent polarity gradients to induce molecular self-assembly, constructing a uniform two-dimensional(2D) perovskite interfacial layer that enables effective defect passivation and rapid charge transport, thereby addressing this trade-off. This strategy achieves a power conversion efficiency (PCE) of 25.72% and a fill factor (FF) of 86.27%, the highest reported values for conventional two-step method-based triple-cation perovskite solar cells (PSCs). Moreover, it demonstrates effectiveness in systems with different passivating agents. This study provides a straightforward and effective approach to improving the efficiency and stability of PSCs.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"284 1","pages":""},"PeriodicalIF":6.475,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146478","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}
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