BACKGROUND Stevens–Johnson syndrome and toxic epidermal necrolysis(SJS/TEN)are very serious skin allergies,with an etiology related to infections and medication.Since the coronavirus disease 2019(COVID-19)pandemic,se...BACKGROUND Stevens–Johnson syndrome and toxic epidermal necrolysis(SJS/TEN)are very serious skin allergies,with an etiology related to infections and medication.Since the coronavirus disease 2019(COVID-19)pandemic,severe acute respiratory syndrome coronavirus-2 has also been considered to cause SJS/TEN.CASE SUMMARY We report the case of a woman in her thirties who took acetaminophen after contracting COVID-19.After 3 d of fever relief,she experienced high fever and presented with SJS/TEN symptoms,accompanied by intrahepatic cholestasis.Three days of corticosteroid treatment did not alleviate the skin damage;therefore,double plasma molecular adsorption system(DPMAS)therapy was initiated,with treatment intervals of 48 h.Her skin symptoms improved gradually and were resolved after seven DPMAS treatments.CONCLUSION DPMAS therapy is beneficial for abrogating SJS/TEN because plasma adsorption and perfusion techniques reduce the inflammatory mediators(e.g.,tumor necrosis factor-alpha and interleukin-10 and-12)speculated to be involved in the pathology of the skin conditions.展开更多
Objective To retrospectively analyze the dual plasma molecular adsorption system(DPMAS)treatment technology and the laboratory data before and after treatment in patients with liver failure and refractory hyperbilirub...Objective To retrospectively analyze the dual plasma molecular adsorption system(DPMAS)treatment technology and the laboratory data before and after treatment in patients with liver failure and refractory hyperbilirubinemia,so as to provide a clinical basis for the prediction1andpreventionof common related complicationsM.I ethods A retrospective study was conducted on 161 cases with liver failure and 683cases with refractory hyperbilirubinemia whounderwent DPMAS treatment in our department from October 2022 to July 2024.The general clinical data characteristics,DPMAS treatment status,DPMAS-related complications,and changes in important laboratory indicators before and after the initial DPMAS treatment in both patient groups were analyzed.Results Among the 229 enrolled cases,82.53%were male,and the median age was 50 years.The cause of liver failure was hepatitis B virus infection in 84.47%,while hepatitis B accounted for only 51.47%in the other group.There were significant differences in platelets,creatinine,coagulation function,and inflammatory factor-related indicators between the two groups at baseline.The total number of DPMAS treatments given was 4471 times.The proportion of albumin used in the initial stage of treatment was significantly higher inpatients with refractory hyperbilirubinemia than that in the liver failure group,while the proportion of plasma used in the liver failure group was significantly higher(P<0.001).The most commonly used anticoagulation regimen was unfractionated heparin.A combined anticoagulation therapy regimen was used in 9.3%of the refractory hyperbilirubinemia group.The internal jugular vein was selected in nearly half of the treated cases.A peripheral vascular access pathway was the treatment option in 31.2%.The proportion of centrifugal separation was significantly higher than that of membrane separation(76.22%vs.23.78%).The incidence rate of DPMAS-related complicationswas 16%.The most common complication was bleeding,including bleeding at the puncture site(accounting for 32%of the total complications)and bleeding at nonpuncture sites(12%),followed by hypotension(22%),allergic reactions(13%)and infections(11%),respectively.The indexes of hemoglobin,platelets,total bilirubin,and C-reactive protein were significantly decreased within 24-48 hours after DPMAS treatment in both groups of patients.The prothrombin time and international normalized ratio were significantly increased in theliver failure group,while fibrinogen was significantly reduced.Conclusion DPMAS clinical application is generally safe in patients with liver disease.The most common complications are bleeding hypotension,allergic reactions,and infections,which need to be paid special attention and timely intervention to ensure the safety profile of treatment.展开更多
Traditional desorption methods in porous sorbents rely heavily on energy-intensive processes such as heating,vacuum pumping,or inert gas purging[1].While effective,these approaches incur substantial energy and operati...Traditional desorption methods in porous sorbents rely heavily on energy-intensive processes such as heating,vacuum pumping,or inert gas purging[1].While effective,these approaches incur substantial energy and operational costs,particularly for hydrocarbons with high boiling points or strong host-vip interactions[2].This is the same case in the newly-developed macrocyclebased crystalline adsorbents,namely nonporous adaptive crystals(NACs).To address these challenges,a recent study published in Angewandte Chemie International Edition by Jie,Ma,and co-workers reported an innovative molecular-"squeeze"triggered desorption mechanism in NACs[3-5].Specifically,ethyl acetate(EA)triggers vip desorption without penetrating the crystal pores or voids.Instead,EA molecules interact with the crystal surface through supramolecular forces,causing the adaptive closure of voids and the subsequent release of vip molecules.Unlike conventional sponges that rely on mechanical squeeze to deform themselves in the bulk for vip release,these macrocycle crystals undergo structural deformation at the molecular level and condensed phase when exposed to vaporized molecules.Because of the similar behavior between sponges and such NACs,the authors name them as sponge-likemacrocyclecrystals.展开更多
Background and Aims:To investigate the safety and efficacy of double plasma molecular adsorption system(DPMAS)with sequential low-dose plasma exchange(LPE)in treating early hepatitis B virus-related acute-on-chronic l...Background and Aims:To investigate the safety and efficacy of double plasma molecular adsorption system(DPMAS)with sequential low-dose plasma exchange(LPE)in treating early hepatitis B virus-related acute-on-chronic liver failure(HBV-ACLF).Methods:Clinical data of patients with HBVACLF were prospectively collected,including patients in a DPMAS with sequential LPE(DPMAS+LPE)group and those in a standard medical treatment(SMT)group.The primary endpoint was death or liver transplantation(LT)at 12 weeks of follow-up.Propensity-score matching was performed to control the effects of confounding factors on prognosis between the two groups.Results:After 2 weeks,total bilirubin,alanine aminotransferase,blood urea nitrogen levels,and Chinese Group on the Study of Severe Hepatitis B score,were significantly lower in the DPMAS+LPE group than those in the SMT group(p<0.05).After 4 weeks,laboratory parameters of the two groups were similar.The cumulative survival rate of the DPMAS+LPE group was significantly higher than that of the SMT group at 4 weeks(97.9%vs.85.4%,p=0.027),but not at 12 weeks(85.4%vs.83.3%,p=0.687).Cytokine levels were significantly lower in 12-week survival group than in the death-or-LT group(p<0.05).Functional enrichment analysis showed that downregulated cytokines were mainly involved in positive regulation of proliferation and activation of lymphocytes and monocytes,regulation of immune effect response,regulation of endotoxin response,and glial cell proliferation.Conclusion:DPMAS+LPE significantly improved the 4-week cumulative survival rate,and ameliorated the inflammatory response in patients.DPMAS+LPE may be a promising modality for patients with early HBV-ACLF.展开更多
Soil and sediment play a crucial role in the fate and transport of perfiuorooctane sulfonate （PFOS） in the environment. However, the molecular mechanisms of major soil/sediment components on PFOS adsorption remain u...Soil and sediment play a crucial role in the fate and transport of perfiuorooctane sulfonate （PFOS） in the environment. However, the molecular mechanisms of major soil/sediment components on PFOS adsorption remain unclear. This study experimentally isolated three major components in soil/sediment： humin/kerogen, humic/fulvic acid （HA/FA）, and inorganic component after removing organics, and explored their contributions to PFOS adsorption using batch adsorption experiments and molecular dynamic simulations. The results suggest that the humin/kerogen component dominated the PFOS adsorption due to its aliphatic features where hydrophobic effect and phase transfer are the primary adsorption mechanism. Compared with the humin/kerogen, the HA/FA component contributed less to the PFOS adsorption because of its hydrophilic and polar characteristics. The electrostatic repulsion between the polar groups of HA/FA and PFOS anions was attributable to the reduced PFOS adsorption. When the soil organic matter was extracted, the inorganic component also plays a non-negligible role because PFOS molecules might form surface complexes on SiO2 surface. The findings obtained in this study illustrate the contribution of organic matters in soils and sediments to PFOS adsorption and provided new perspective to understanding the adsorption process of PFOS on micro-interface in the environment.展开更多
The Grand Canonical Monte Carlo(GCMC) simulation method was used to investigate the adsorption properties of quinoline homologues(quinoline, 2-methyl quinoline, and 2,4-dimethyl quinoline) on the FAU zeolite. The adso...The Grand Canonical Monte Carlo(GCMC) simulation method was used to investigate the adsorption properties of quinoline homologues(quinoline, 2-methyl quinoline, and 2,4-dimethyl quinoline) on the FAU zeolite. The adsorption heat, adsorption isotherms, and adsorption sites of them were obtained. At the temperature ranging from 673.15 to 873.15 K, the Henry constant of quinoline homologues calculated on the FAU zeolite was applied to simulate their adsorption heat. And its value was more in accordance with the related data reported in the literature. The results showed that their isosteric heat decreased in the following order: 2,4-dimethyl quinoline(118.63 kJ/mol) > 2-methyl quinoline(110.45 kJ/mol) > quinoline(98 kJ/mol), and complied with the order of their adsorbate basicity. The competitive adsorption of three components of quinoline homologues on the FAU zeolite was calculated numerically at a temperature of 773.15 K and a pressure range of 0.1—100 MPa under the Universal force field. Their adsorption capacity decreased in the following order: quinoline > 2-methyl quinoline > 2,4-dimethyl quinoline. The smaller the molecule size of the adsorbate, the greater the saturated adsorption capacity would be. It was found that the quinoline homologues could be adsorbed in the main channels of 12- membered-ring framework of the zeolite. Simultaneously, the influence of silica/alumina ratio on the adsorption property of quinoline homologues in FAU zeolite was studied. The smaller the silica/alumina ratio, the greater the isosteric heat and adsorption capacity would be.展开更多
Adsorption of FCC dry gas components, hydrogen(H_2), nitrogen(N_2), methane(CH_4), ethane(C_2H_6) and ethylene(C_2H_4) in zeolite Y was studied by performing the Grant Canonical Monte Carlo(GCMC) simulations at 298K a...Adsorption of FCC dry gas components, hydrogen(H_2), nitrogen(N_2), methane(CH_4), ethane(C_2H_6) and ethylene(C_2H_4) in zeolite Y was studied by performing the Grant Canonical Monte Carlo(GCMC) simulations at 298K and 823K and under a pressure range up to 10 MPa. Simulation results were analyzed using the Langmuir model, which presented fitting of dry gas components adsorption to be suggested as the monolayer adsorption. C_2H_4 presented most single adsorption amount, which reached 7.63 mol/kg at 298K under a pressure of 200kPa. Thermodynamic parameters of the Gibbs free energy change, enthalpy change and entropy change were analyzed based on adsorption equilibrium constant obtained from the GCMC simulations. The results suggested that it was more favorable for C_2H_4 to be adsorbed in zeolite Y. Adsorption molecules were in ordered arrangement in the zeolite, and C_2H_4 exhibited a more orderly arrangement than other components. Additionally, a competition in the adsorption of a mixture of dry gas components was found, and supercages were the priority adsorption space. The competition was favorable to CH_4 and C_2H_6, and the competitive power was affected by temperature.展开更多
CO adsorption on small Aun （n = 1 - 7） clusters which are supported by a partially reduced rutile TiO2（110） surface has been investigated by the first-principles method. The low coordinated sites of Au clusters ar...CO adsorption on small Aun （n = 1 - 7） clusters which are supported by a partially reduced rutile TiO2（110） surface has been investigated by the first-principles method. The low coordinated sites of Au clusters are favorable for CO adsorption. CO-Aun-TiO2 system displays surface magnetism. There is a strong interaction between the adsorbed CO molecule and the supported Au clusters.展开更多
Since the capacity of CO2 adsorption of coal is a key factor in coal and CO2 outbursts,an experimental study was carried out on CO2 isothermal adsorption with high-pressure volumetry with dry coal samples from the No....Since the capacity of CO2 adsorption of coal is a key factor in coal and CO2 outbursts,an experimental study was carried out on CO2 isothermal adsorption with high-pressure volumetry with dry coal samples from the No.2 coal seam in the Haishiwan Coalfield.Four different equations(Langmuir,BET,D-R and D-A) were used to fit the experimental data.We discuss adsorption mechanisms.The results show that the amount of CO2 adsorption increases rapidly under low relative pressure,i.e.,the ratio of equilibrium pressure and saturated vapor pressure,which indicates that molecular layer adsorption or micropore filling may occur in coal.No clear equilibrium state was observed on the isothermal adsorption curves under relative pressure(P /P0 ) ranging from 0 to 0.8.The fitted results show that the accuracy of the D-A equation is highest with n=1.Micropores are more developed in coal by comparing the BET equation with a pressure mercury injection method on the surface area.The D-A equation(n=1) provides the best fit.By comparing the calculated specific surface area of the BET equation and the mercury intrusion method,it is found that micropore adsorption of CO2 occupies a dominant position.展开更多
The paper presents a Monte Carlo simulation to study the adsorption characteristics of methane molecule on coal slit pores from different aspects.Firstly,a physical model of adsorption and desorption of methane molecu...The paper presents a Monte Carlo simulation to study the adsorption characteristics of methane molecule on coal slit pores from different aspects.Firstly,a physical model of adsorption and desorption of methane molecules on micropores was established.Secondly,a grand canonical ensemble was introduced as the Monte Carlo simulation system.Thirdly,based on the model and system,the molecule simulation program was developed with VC++6.0 to simulate the isothermal adsorption relationship between the amount of molecule absorption and the factors affecting it.Lastly,the numerically simulated results were compared with measured results of adsorption coal samples of two different coal mines with a laboratory gas absorption instrument.The results show that the molecule simulations of the adsorption constants,the adsorption quantity,and the isothermal adsorption curve at the same and different coal temperatures were in good agreement with those measured in the experiments,indicating that it is feasible to use the established model and the Monte Carlo molecule simulation to study the adsorption characteristics of methane molecules in coal.展开更多
Using density functional theory, noncovalent interactions and two mechanisms of covalent functionalization of drug carmustine with functionalized carbon nanotube（CNT） have been investigated. Quantum molecular descri...Using density functional theory, noncovalent interactions and two mechanisms of covalent functionalization of drug carmustine with functionalized carbon nanotube（CNT） have been investigated. Quantum molecular descriptors of noncovalent configurations were studied. It was specified that binding of drug carmustine with functionalized CNT is thermodynamically suitable. NTCOOH and NTCOCl can bond to the NH group of carmustine through OH（COOH mechanism） and Cl（COCl mechanism） groups, respectively. The activation energies, activation enthalpies and activation Gibbs free energies of two pathways were calculated and compared with each other. The activation parameters related to COOH mechanism are higher than those related to COCl mechanism, and therefore COCl mechanism is suitable for covalent functionalization. COOH functionalized CNT（NTCOOH） has more binding energy than COCl functionalized CNT（NTCOCl） and can act as a favorable system for carmustine drug delivery within biological and chemical systems（noncovalent）. These results could be generalized to other similar drugs.展开更多
Molecular imprinted polymers (MIPs) are novel functional polymer materials and known as specific adsorbents for the template molecules. These novel functional polymers have promised potential applications in racemic r...Molecular imprinted polymers (MIPs) are novel functional polymer materials and known as specific adsorbents for the template molecules. These novel functional polymers have promised potential applications in racemic resolution, sensor, chromatography, adsorptive separation and other fields. This review exhibits the approach for preparing MIPs, the features of MIPs obtained by different routes and the characteristics of adsorptive separations with MIPs. The molecular recognition mechanism and the idea of the present possibilities and limitations of molecular imprinting polymerization are discussed as well.展开更多
In the field of catalytic hydro-genation,two primary mecha-nistic pathways,namely the Ho-riuti-Polanyi(HP)mechanism and the non-HP mechanism,have been extensively investi-gated.Current understandings suggested that th...In the field of catalytic hydro-genation,two primary mecha-nistic pathways,namely the Ho-riuti-Polanyi(HP)mechanism and the non-HP mechanism,have been extensively investi-gated.Current understandings suggested that the non-HP mechanism preferred to occur on the coinage metal surfaces,such as copper,silver,and gold,which exhibited low activity towards H_(2) dissociation.Herein,we offered a detailed theoretical investigation into the mechanisms of CO_(2)hydrogenation to formic acid on M_(1)-In_(2)O_(3)(111)surfaces,using density functional theory calculations.Our calculations provided novel in-sights into the preference of the non-HP mechanism on reduced single-atom noble metal cata-lysts,such as r-Rh_(1)-In_(2)O_(3)(111)and r-Ir_(1)-In_(2)O_(3)(111).In these cases,molecularly adsorbed H_(2) would be polarized into H^(δ−)-H^(δ+),thus facilitating the electrophilic attack to the O in CO_(2).Conversely,the H^(δ+)species,derived from heterolytically dissociated H_(2),exhibited a strong affinity on the adjacent oxygen site at the M-O-In interface.This strong adsorption resulted in a higher energy barrier for CO_(2)hydrogenation,thereby rendering the HP mechanism less viable than the non-HP one.Our results were anticipated to provide a deeper understanding of hydrogenation reactions on oxide-supported noble single-atom catalysts and theoretical guidance for the development of novel high-performance catalysts for catalytic hydrogena-tion reactions.展开更多
BACKGROUND Immune checkpoint inhibitors(ICIs)can lead to immune-related hepatitis(IRH)and severe liver damage,which is life-threatening in the absence of specific treatment.CASE SUMMARY A 75-year-old man was admitted ...BACKGROUND Immune checkpoint inhibitors(ICIs)can lead to immune-related hepatitis(IRH)and severe liver damage,which is life-threatening in the absence of specific treatment.CASE SUMMARY A 75-year-old man was admitted to our hospital complaining of loss of appetite,yellow urine,and abnormal liver function for the past 2 wk.Three months prior to admission,he was treated with two rounds of capecitabine in combination with camrelizumab for lymph node metastasis of esophageal cancer.Although liver function was normal before treatment,abnormal liver function appeared at week 5.Capecitabine and camrelizumab were discontinued.Ursodeoxycholic acid and methylprednisolone 40 mg daily were administered.Liver function continued to deteriorate.Prothrombin time and international normalized ratio were 19 s and 1.8,respectively.The patient was diagnosed with acute liver failure.A pathological analysis of liver biopsy indicated a strongly positive immunohistochemical staining of T8+cells,thereby suggesting that drug-induced liver injury was related to IRH caused by camrelizumab.Subsequently,we performed sequential dual-molecule plasma adsorption system(DPMAS)treatment with plasma exchange(PE).After two rounds of treatment,the patient's appetite significantly improved,the yellow color of urine reduced,and liver function improved(total bilirubin level decreased)after five rounds of treatment.Liver function normalized 4 wk after discharge.CONCLUSION The use of sequential DPMAS with PE can reduce liver injury and systemic toxic reactions by clearing inflammatory mediators and harmful substances from blood,and regulate immune cell activity,which may be effective in the treatment of severe ICI-induced IRH.展开更多
The acid number of the mixed solution of 150SN oil and oleic acid characterizes the volume content of oleic acid in the solution,based on which the adsorptive capability of oleic acid is studied on the 45 steel balls ...The acid number of the mixed solution of 150SN oil and oleic acid characterizes the volume content of oleic acid in the solution,based on which the adsorptive capability of oleic acid is studied on the 45 steel balls and disks.Boundary lubrication tests are carried out on a self designed ball-on-disk machine,The base oil is pure 150SN oil,and oleic acid as additive are added into the lubricant.Disks have surface roughness values(Ra)of 0.8μn and 0.4μn.The electrical contact resistance method is used to determine the lubrication status.Hypothesize that the molecular film is monomolecular layer in condensed state and the opposing surfaces are completely separated by molecular film.A boundary lubrication model is established according to experimental results and hypothesizes.The experimental and calculatienal results show that the adsorption of polar molecules on steel surface is the main factor to form the boundary lubrication film.Load and sliding speed contribute little to the friction coefficient of boundary lubrication.The properties of steel surface and additive for the lubricant significantly influence on the characters of boundary lubrication.The smaller the surface roughness value is,the smaller the friction coefficient of the boundary lubrication is.展开更多
Based on the generalized gradient approximation （GGA）, Perdew-Wang-91 （PW91） combined with a periodic slab model has been applied to study the catalytic activity of chlorine evolution on TinRumO2 （1 1 0） surface...Based on the generalized gradient approximation （GGA）, Perdew-Wang-91 （PW91） combined with a periodic slab model has been applied to study the catalytic activity of chlorine evolution on TinRumO2 （1 1 0） surface. Metal oxide model TinRumO2 has been established with pure TiO2 and Ru02 on the basis set of Double Numerical plus polarization （DNP）, in which the proportion of n：m was 3：1, 1 ：l, or 1：3. Analysis on the reaction activity in the electrochemical reaction and the electrochemical desorption reaction was based on Frontier molecular orbital theory. The results show that the TinRumO2 with a ratio of Ti：Ru at 3：1 is best facilitates the electrochemical reaction and electrochemical desorption reaction to produce M-Clads intermediate and precipitate C12. In addition, the adsorption energy of Cl on the surface of Ti3RU102 possesses the minimum value of 2.514 eV, and thus electrochemical desorption reaction could occur most easily.展开更多
The single thiolated arylethynylene molecule with 9,10-dihydroanthracene core（denoted as TADHA） possesses pronounced negative differential conductance（NDC） behavior at lower bias regime. The adsorption effects of ...The single thiolated arylethynylene molecule with 9,10-dihydroanthracene core（denoted as TADHA） possesses pronounced negative differential conductance（NDC） behavior at lower bias regime. The adsorption effects of F2 molecule on the current and NDC behavior of TADHA molecular junctions are studied by applying non-equilibrium Green＇s formalism combined with density functional theory. The numerical results show that the F2 molecule adsorbed on the benzene ring of TADHA molecule near the electrode can dramatically suppresses the current of TADHA molecular junction. When the F2 molecule adsorbed on the conjugated segment of 9,10-dihydroanthracene core of TADHA molecule, an obviously asymmetric effect on the current curves induces the molecular system showing apparent rectifier behavior. However, the current especially the NDC behavior have been significantly enlarged when F2 addition reacted with triple bond of TADHA molecule.展开更多
Metal-organic frameworks(MOFs)have long been highly regarded for their crystalline order,structural modularity,and precisely defined porosity.Metal nodes and organic linkers form ordered lattices with defined pores,en...Metal-organic frameworks(MOFs)have long been highly regarded for their crystalline order,structural modularity,and precisely defined porosity.Metal nodes and organic linkers form ordered lattices with defined pores,enabling predictable adsorp-tion and transport processes.Traditionally,research on MOFs has primarily focused on established fields such as molecular adsorption and heterogeneous catalysis[1,2]展开更多
Here we present a combined DFF and molecular dynamics study of uranyl （U（VI）） interaction mecha- nisms with the calcite （104） surface in aqueous solution. The roles of three anion ligands （CO2 , HCO3, OH ） and...Here we present a combined DFF and molecular dynamics study of uranyl （U（VI）） interaction mecha- nisms with the calcite （104） surface in aqueous solution. The roles of three anion ligands （CO2 , HCO3, OH ） and solvation effect in U（VI） interaction with calcite have been evaluated. According to our calculations, water adsorbed on the calcite （104） surface prefers to exist in molecular state rather than dis- sociative state. Energy analysis indicate that the positively charged uranyl species prefers to form surface complexes on the surface, while neutral uranyl species may bind with the surface via both surface complexing and ion exchange reactions of U（VI） → Ca（II）. In contrast, the negatively charged uranyl species prefer to interact with the surface via ion exchange reactions of U（VI）→ Ca（II）, and the one with UO2（CO3）2（H2O）^2- as the reactant becomes the most favorable one in energy. We also found that uranyl adsorption increases the hydrophilicability of the （104） surface to different extents, where the UO2（CO3）3Ca2 species contributes to the largest degree of energy changes （ 53 kcal/mol）. Our calcula- tions proved that the （104） surface also has the ability to immobilize U（VI） via either surface complexing or ion exchange mechanisms under different pH values.展开更多
The pressing challenges of the energy crisis and environmental problems necessitate the pursuit of efficient and sustainable energy conversion technologies,wherein catalytic processes play a vital role in addressing t...The pressing challenges of the energy crisis and environmental problems necessitate the pursuit of efficient and sustainable energy conversion technologies,wherein catalytic processes play a vital role in addressing these issues.Single-molecule fluorescence microscopy(SMFM)offers a transformative approach to understanding various catalytic reactions by enabling real-time visualization of molecular adsorption,diffusion,and transformation on catalytic surfaces.The unprecedented insights into the spatial distribution of active sites,catalytic heterogeneity,and the dynamics of key intermediates result in single-or subparticle level structure−property relations,thereby offering insightful perspectives for catalyst design and mechanistic understanding of energy-related catalytic processes.In this review,we provide an overview of the recent progress in using SMFM for investigating energy-related catalytic reactions.The advancement in SMFM imaging techniques for investigating nonfluorescent chemical processes is also highlighted.Finally,we conclude the review by commenting on the current challenges and prospects in advancing SMFM in energy research.We hope that the capable SMFM imaging techniques and insights will promote the development and realistic application of various energy-related catalytic reactions,together with inspiring researchers to explore the power of SMFM in other applications.展开更多
文摘BACKGROUND Stevens–Johnson syndrome and toxic epidermal necrolysis(SJS/TEN)are very serious skin allergies,with an etiology related to infections and medication.Since the coronavirus disease 2019(COVID-19)pandemic,severe acute respiratory syndrome coronavirus-2 has also been considered to cause SJS/TEN.CASE SUMMARY We report the case of a woman in her thirties who took acetaminophen after contracting COVID-19.After 3 d of fever relief,she experienced high fever and presented with SJS/TEN symptoms,accompanied by intrahepatic cholestasis.Three days of corticosteroid treatment did not alleviate the skin damage;therefore,double plasma molecular adsorption system(DPMAS)therapy was initiated,with treatment intervals of 48 h.Her skin symptoms improved gradually and were resolved after seven DPMAS treatments.CONCLUSION DPMAS therapy is beneficial for abrogating SJS/TEN because plasma adsorption and perfusion techniques reduce the inflammatory mediators(e.g.,tumor necrosis factor-alpha and interleukin-10 and-12)speculated to be involved in the pathology of the skin conditions.
文摘Objective To retrospectively analyze the dual plasma molecular adsorption system(DPMAS)treatment technology and the laboratory data before and after treatment in patients with liver failure and refractory hyperbilirubinemia,so as to provide a clinical basis for the prediction1andpreventionof common related complicationsM.I ethods A retrospective study was conducted on 161 cases with liver failure and 683cases with refractory hyperbilirubinemia whounderwent DPMAS treatment in our department from October 2022 to July 2024.The general clinical data characteristics,DPMAS treatment status,DPMAS-related complications,and changes in important laboratory indicators before and after the initial DPMAS treatment in both patient groups were analyzed.Results Among the 229 enrolled cases,82.53%were male,and the median age was 50 years.The cause of liver failure was hepatitis B virus infection in 84.47%,while hepatitis B accounted for only 51.47%in the other group.There were significant differences in platelets,creatinine,coagulation function,and inflammatory factor-related indicators between the two groups at baseline.The total number of DPMAS treatments given was 4471 times.The proportion of albumin used in the initial stage of treatment was significantly higher inpatients with refractory hyperbilirubinemia than that in the liver failure group,while the proportion of plasma used in the liver failure group was significantly higher(P<0.001).The most commonly used anticoagulation regimen was unfractionated heparin.A combined anticoagulation therapy regimen was used in 9.3%of the refractory hyperbilirubinemia group.The internal jugular vein was selected in nearly half of the treated cases.A peripheral vascular access pathway was the treatment option in 31.2%.The proportion of centrifugal separation was significantly higher than that of membrane separation(76.22%vs.23.78%).The incidence rate of DPMAS-related complicationswas 16%.The most common complication was bleeding,including bleeding at the puncture site(accounting for 32%of the total complications)and bleeding at nonpuncture sites(12%),followed by hypotension(22%),allergic reactions(13%)and infections(11%),respectively.The indexes of hemoglobin,platelets,total bilirubin,and C-reactive protein were significantly decreased within 24-48 hours after DPMAS treatment in both groups of patients.The prothrombin time and international normalized ratio were significantly increased in theliver failure group,while fibrinogen was significantly reduced.Conclusion DPMAS clinical application is generally safe in patients with liver disease.The most common complications are bleeding hypotension,allergic reactions,and infections,which need to be paid special attention and timely intervention to ensure the safety profile of treatment.
基金the Natural Science Foundation of Jiangsu Province(No.BK20240679)National Natural Science Foundation of China(No.22101134)are greatly acknowledged。
文摘Traditional desorption methods in porous sorbents rely heavily on energy-intensive processes such as heating,vacuum pumping,or inert gas purging[1].While effective,these approaches incur substantial energy and operational costs,particularly for hydrocarbons with high boiling points or strong host-vip interactions[2].This is the same case in the newly-developed macrocyclebased crystalline adsorbents,namely nonporous adaptive crystals(NACs).To address these challenges,a recent study published in Angewandte Chemie International Edition by Jie,Ma,and co-workers reported an innovative molecular-"squeeze"triggered desorption mechanism in NACs[3-5].Specifically,ethyl acetate(EA)triggers vip desorption without penetrating the crystal pores or voids.Instead,EA molecules interact with the crystal surface through supramolecular forces,causing the adaptive closure of voids and the subsequent release of vip molecules.Unlike conventional sponges that rely on mechanical squeeze to deform themselves in the bulk for vip release,these macrocycle crystals undergo structural deformation at the molecular level and condensed phase when exposed to vaporized molecules.Because of the similar behavior between sponges and such NACs,the authors name them as sponge-likemacrocyclecrystals.
基金This study was supported by grants from the National major science and technology project for the prevention and treatment of AIDS and viral hepatitis(2018ZX10302204-002-002 to LP,2018ZX10302205-002 to CX)Natural Science Foundation of China(No.81873572 to LP,82070611 to LP)+3 种基金Guangzhou Science and Technology Plan Projects(201904010442 to CX,202102010204 to LP)Guangdong Science and Technology Plan Projects(2020A1515010317 to CX)Sun Yat-Sen University Clinical Research 5010 Program(2018009 to CX,2020007 to LP)the Five-Year Plan of Third Affiliated Hospital of Sun Yat-Sen University(K00006 to LP).
文摘Background and Aims:To investigate the safety and efficacy of double plasma molecular adsorption system(DPMAS)with sequential low-dose plasma exchange(LPE)in treating early hepatitis B virus-related acute-on-chronic liver failure(HBV-ACLF).Methods:Clinical data of patients with HBVACLF were prospectively collected,including patients in a DPMAS with sequential LPE(DPMAS+LPE)group and those in a standard medical treatment(SMT)group.The primary endpoint was death or liver transplantation(LT)at 12 weeks of follow-up.Propensity-score matching was performed to control the effects of confounding factors on prognosis between the two groups.Results:After 2 weeks,total bilirubin,alanine aminotransferase,blood urea nitrogen levels,and Chinese Group on the Study of Severe Hepatitis B score,were significantly lower in the DPMAS+LPE group than those in the SMT group(p<0.05).After 4 weeks,laboratory parameters of the two groups were similar.The cumulative survival rate of the DPMAS+LPE group was significantly higher than that of the SMT group at 4 weeks(97.9%vs.85.4%,p=0.027),but not at 12 weeks(85.4%vs.83.3%,p=0.687).Cytokine levels were significantly lower in 12-week survival group than in the death-or-LT group(p<0.05).Functional enrichment analysis showed that downregulated cytokines were mainly involved in positive regulation of proliferation and activation of lymphocytes and monocytes,regulation of immune effect response,regulation of endotoxin response,and glial cell proliferation.Conclusion:DPMAS+LPE significantly improved the 4-week cumulative survival rate,and ameliorated the inflammatory response in patients.DPMAS+LPE may be a promising modality for patients with early HBV-ACLF.
基金supported by the National Basic Research Program (973) of China (No. 2014CB441102)the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB14020201)Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences (No. YSW2013A01)
文摘Soil and sediment play a crucial role in the fate and transport of perfiuorooctane sulfonate （PFOS） in the environment. However, the molecular mechanisms of major soil/sediment components on PFOS adsorption remain unclear. This study experimentally isolated three major components in soil/sediment： humin/kerogen, humic/fulvic acid （HA/FA）, and inorganic component after removing organics, and explored their contributions to PFOS adsorption using batch adsorption experiments and molecular dynamic simulations. The results suggest that the humin/kerogen component dominated the PFOS adsorption due to its aliphatic features where hydrophobic effect and phase transfer are the primary adsorption mechanism. Compared with the humin/kerogen, the HA/FA component contributed less to the PFOS adsorption because of its hydrophilic and polar characteristics. The electrostatic repulsion between the polar groups of HA/FA and PFOS anions was attributable to the reduced PFOS adsorption. When the soil organic matter was extracted, the inorganic component also plays a non-negligible role because PFOS molecules might form surface complexes on SiO2 surface. The findings obtained in this study illustrate the contribution of organic matters in soils and sediments to PFOS adsorption and provided new perspective to understanding the adsorption process of PFOS on micro-interface in the environment.
文摘The Grand Canonical Monte Carlo(GCMC) simulation method was used to investigate the adsorption properties of quinoline homologues(quinoline, 2-methyl quinoline, and 2,4-dimethyl quinoline) on the FAU zeolite. The adsorption heat, adsorption isotherms, and adsorption sites of them were obtained. At the temperature ranging from 673.15 to 873.15 K, the Henry constant of quinoline homologues calculated on the FAU zeolite was applied to simulate their adsorption heat. And its value was more in accordance with the related data reported in the literature. The results showed that their isosteric heat decreased in the following order: 2,4-dimethyl quinoline(118.63 kJ/mol) > 2-methyl quinoline(110.45 kJ/mol) > quinoline(98 kJ/mol), and complied with the order of their adsorbate basicity. The competitive adsorption of three components of quinoline homologues on the FAU zeolite was calculated numerically at a temperature of 773.15 K and a pressure range of 0.1—100 MPa under the Universal force field. Their adsorption capacity decreased in the following order: quinoline > 2-methyl quinoline > 2,4-dimethyl quinoline. The smaller the molecule size of the adsorbate, the greater the saturated adsorption capacity would be. It was found that the quinoline homologues could be adsorbed in the main channels of 12- membered-ring framework of the zeolite. Simultaneously, the influence of silica/alumina ratio on the adsorption property of quinoline homologues in FAU zeolite was studied. The smaller the silica/alumina ratio, the greater the isosteric heat and adsorption capacity would be.
基金financial support from the National Natural Science Foundation of China (No. 41302101 and No. 21476263)
文摘Adsorption of FCC dry gas components, hydrogen(H_2), nitrogen(N_2), methane(CH_4), ethane(C_2H_6) and ethylene(C_2H_4) in zeolite Y was studied by performing the Grant Canonical Monte Carlo(GCMC) simulations at 298K and 823K and under a pressure range up to 10 MPa. Simulation results were analyzed using the Langmuir model, which presented fitting of dry gas components adsorption to be suggested as the monolayer adsorption. C_2H_4 presented most single adsorption amount, which reached 7.63 mol/kg at 298K under a pressure of 200kPa. Thermodynamic parameters of the Gibbs free energy change, enthalpy change and entropy change were analyzed based on adsorption equilibrium constant obtained from the GCMC simulations. The results suggested that it was more favorable for C_2H_4 to be adsorbed in zeolite Y. Adsorption molecules were in ordered arrangement in the zeolite, and C_2H_4 exhibited a more orderly arrangement than other components. Additionally, a competition in the adsorption of a mixture of dry gas components was found, and supercages were the priority adsorption space. The competition was favorable to CH_4 and C_2H_6, and the competitive power was affected by temperature.
基金supported by the National Natural Science Foundation of China (Grant No. 10604035)the National Basic Research Program of China (Grant No. 2006CB605102)
文摘CO adsorption on small Aun （n = 1 - 7） clusters which are supported by a partially reduced rutile TiO2（110） surface has been investigated by the first-principles method. The low coordinated sites of Au clusters are favorable for CO adsorption. CO-Aun-TiO2 system displays surface magnetism. There is a strong interaction between the adsorbed CO molecule and the supported Au clusters.
基金the National Basic Research Program of China (No.2005CB221503)the Major Program of the National Natural Science Foundation (Nos.70533050 and 50674089) for their support of this project
文摘Since the capacity of CO2 adsorption of coal is a key factor in coal and CO2 outbursts,an experimental study was carried out on CO2 isothermal adsorption with high-pressure volumetry with dry coal samples from the No.2 coal seam in the Haishiwan Coalfield.Four different equations(Langmuir,BET,D-R and D-A) were used to fit the experimental data.We discuss adsorption mechanisms.The results show that the amount of CO2 adsorption increases rapidly under low relative pressure,i.e.,the ratio of equilibrium pressure and saturated vapor pressure,which indicates that molecular layer adsorption or micropore filling may occur in coal.No clear equilibrium state was observed on the isothermal adsorption curves under relative pressure(P /P0 ) ranging from 0 to 0.8.The fitted results show that the accuracy of the D-A equation is highest with n=1.Micropores are more developed in coal by comparing the BET equation with a pressure mercury injection method on the surface area.The D-A equation(n=1) provides the best fit.By comparing the calculated specific surface area of the BET equation and the mercury intrusion method,it is found that micropore adsorption of CO2 occupies a dominant position.
基金supported by the Industrial Research Project in Guizhou Science and Technology Bureau of China (GY(2011)No.3012)International Cooperation Projects in Guizhou Science and Technology Bureau of China (G(2009)No.700111)
文摘The paper presents a Monte Carlo simulation to study the adsorption characteristics of methane molecule on coal slit pores from different aspects.Firstly,a physical model of adsorption and desorption of methane molecules on micropores was established.Secondly,a grand canonical ensemble was introduced as the Monte Carlo simulation system.Thirdly,based on the model and system,the molecule simulation program was developed with VC++6.0 to simulate the isothermal adsorption relationship between the amount of molecule absorption and the factors affecting it.Lastly,the numerically simulated results were compared with measured results of adsorption coal samples of two different coal mines with a laboratory gas absorption instrument.The results show that the molecule simulations of the adsorption constants,the adsorption quantity,and the isothermal adsorption curve at the same and different coal temperatures were in good agreement with those measured in the experiments,indicating that it is feasible to use the established model and the Monte Carlo molecule simulation to study the adsorption characteristics of methane molecules in coal.
文摘Using density functional theory, noncovalent interactions and two mechanisms of covalent functionalization of drug carmustine with functionalized carbon nanotube（CNT） have been investigated. Quantum molecular descriptors of noncovalent configurations were studied. It was specified that binding of drug carmustine with functionalized CNT is thermodynamically suitable. NTCOOH and NTCOCl can bond to the NH group of carmustine through OH（COOH mechanism） and Cl（COCl mechanism） groups, respectively. The activation energies, activation enthalpies and activation Gibbs free energies of two pathways were calculated and compared with each other. The activation parameters related to COOH mechanism are higher than those related to COCl mechanism, and therefore COCl mechanism is suitable for covalent functionalization. COOH functionalized CNT（NTCOOH） has more binding energy than COCl functionalized CNT（NTCOCl） and can act as a favorable system for carmustine drug delivery within biological and chemical systems（noncovalent）. These results could be generalized to other similar drugs.
文摘Molecular imprinted polymers (MIPs) are novel functional polymer materials and known as specific adsorbents for the template molecules. These novel functional polymers have promised potential applications in racemic resolution, sensor, chromatography, adsorptive separation and other fields. This review exhibits the approach for preparing MIPs, the features of MIPs obtained by different routes and the characteristics of adsorptive separations with MIPs. The molecular recognition mechanism and the idea of the present possibilities and limitations of molecular imprinting polymerization are discussed as well.
基金supported by the National Key Research and Development Program of Ministry of Sci-ence and Technology of China(No.2022YFA1504601)the National Natural Science Foundation of China(Nos.92045303,22132004,22121001,22072116,22072117,and 21773192).
文摘In the field of catalytic hydro-genation,two primary mecha-nistic pathways,namely the Ho-riuti-Polanyi(HP)mechanism and the non-HP mechanism,have been extensively investi-gated.Current understandings suggested that the non-HP mechanism preferred to occur on the coinage metal surfaces,such as copper,silver,and gold,which exhibited low activity towards H_(2) dissociation.Herein,we offered a detailed theoretical investigation into the mechanisms of CO_(2)hydrogenation to formic acid on M_(1)-In_(2)O_(3)(111)surfaces,using density functional theory calculations.Our calculations provided novel in-sights into the preference of the non-HP mechanism on reduced single-atom noble metal cata-lysts,such as r-Rh_(1)-In_(2)O_(3)(111)and r-Ir_(1)-In_(2)O_(3)(111).In these cases,molecularly adsorbed H_(2) would be polarized into H^(δ−)-H^(δ+),thus facilitating the electrophilic attack to the O in CO_(2).Conversely,the H^(δ+)species,derived from heterolytically dissociated H_(2),exhibited a strong affinity on the adjacent oxygen site at the M-O-In interface.This strong adsorption resulted in a higher energy barrier for CO_(2)hydrogenation,thereby rendering the HP mechanism less viable than the non-HP one.Our results were anticipated to provide a deeper understanding of hydrogenation reactions on oxide-supported noble single-atom catalysts and theoretical guidance for the development of novel high-performance catalysts for catalytic hydrogena-tion reactions.
文摘BACKGROUND Immune checkpoint inhibitors(ICIs)can lead to immune-related hepatitis(IRH)and severe liver damage,which is life-threatening in the absence of specific treatment.CASE SUMMARY A 75-year-old man was admitted to our hospital complaining of loss of appetite,yellow urine,and abnormal liver function for the past 2 wk.Three months prior to admission,he was treated with two rounds of capecitabine in combination with camrelizumab for lymph node metastasis of esophageal cancer.Although liver function was normal before treatment,abnormal liver function appeared at week 5.Capecitabine and camrelizumab were discontinued.Ursodeoxycholic acid and methylprednisolone 40 mg daily were administered.Liver function continued to deteriorate.Prothrombin time and international normalized ratio were 19 s and 1.8,respectively.The patient was diagnosed with acute liver failure.A pathological analysis of liver biopsy indicated a strongly positive immunohistochemical staining of T8+cells,thereby suggesting that drug-induced liver injury was related to IRH caused by camrelizumab.Subsequently,we performed sequential dual-molecule plasma adsorption system(DPMAS)treatment with plasma exchange(PE).After two rounds of treatment,the patient's appetite significantly improved,the yellow color of urine reduced,and liver function improved(total bilirubin level decreased)after five rounds of treatment.Liver function normalized 4 wk after discharge.CONCLUSION The use of sequential DPMAS with PE can reduce liver injury and systemic toxic reactions by clearing inflammatory mediators and harmful substances from blood,and regulate immune cell activity,which may be effective in the treatment of severe ICI-induced IRH.
基金This project is supported by Specialized Research Fund for Doctoral Program of Higher Education,China(No.20030561007)
文摘The acid number of the mixed solution of 150SN oil and oleic acid characterizes the volume content of oleic acid in the solution,based on which the adsorptive capability of oleic acid is studied on the 45 steel balls and disks.Boundary lubrication tests are carried out on a self designed ball-on-disk machine,The base oil is pure 150SN oil,and oleic acid as additive are added into the lubricant.Disks have surface roughness values(Ra)of 0.8μn and 0.4μn.The electrical contact resistance method is used to determine the lubrication status.Hypothesize that the molecular film is monomolecular layer in condensed state and the opposing surfaces are completely separated by molecular film.A boundary lubrication model is established according to experimental results and hypothesizes.The experimental and calculatienal results show that the adsorption of polar molecules on steel surface is the main factor to form the boundary lubrication film.Load and sliding speed contribute little to the friction coefficient of boundary lubrication.The properties of steel surface and additive for the lubricant significantly influence on the characters of boundary lubrication.The smaller the surface roughness value is,the smaller the friction coefficient of the boundary lubrication is.
基金the Natural Science Foundation of China(No. 51072239)the Fundamental Research Funds for the Central Universities(No.CQDXWL-2012-032) for financial support
文摘Based on the generalized gradient approximation （GGA）, Perdew-Wang-91 （PW91） combined with a periodic slab model has been applied to study the catalytic activity of chlorine evolution on TinRumO2 （1 1 0） surface. Metal oxide model TinRumO2 has been established with pure TiO2 and Ru02 on the basis set of Double Numerical plus polarization （DNP）, in which the proportion of n：m was 3：1, 1 ：l, or 1：3. Analysis on the reaction activity in the electrochemical reaction and the electrochemical desorption reaction was based on Frontier molecular orbital theory. The results show that the TinRumO2 with a ratio of Ti：Ru at 3：1 is best facilitates the electrochemical reaction and electrochemical desorption reaction to produce M-Clads intermediate and precipitate C12. In addition, the adsorption energy of Cl on the surface of Ti3RU102 possesses the minimum value of 2.514 eV, and thus electrochemical desorption reaction could occur most easily.
基金Project supported by the National Natural Science Foundation of China(Grant No.11374195)the Taishan Scholar Project of Shandong Province,Chinathe Jinan Youth Science and Technology Star Project,China(Grant No.201406004)
文摘The single thiolated arylethynylene molecule with 9,10-dihydroanthracene core（denoted as TADHA） possesses pronounced negative differential conductance（NDC） behavior at lower bias regime. The adsorption effects of F2 molecule on the current and NDC behavior of TADHA molecular junctions are studied by applying non-equilibrium Green＇s formalism combined with density functional theory. The numerical results show that the F2 molecule adsorbed on the benzene ring of TADHA molecule near the electrode can dramatically suppresses the current of TADHA molecular junction. When the F2 molecule adsorbed on the conjugated segment of 9,10-dihydroanthracene core of TADHA molecule, an obviously asymmetric effect on the current curves induces the molecular system showing apparent rectifier behavior. However, the current especially the NDC behavior have been significantly enlarged when F2 addition reacted with triple bond of TADHA molecule.
文摘Metal-organic frameworks(MOFs)have long been highly regarded for their crystalline order,structural modularity,and precisely defined porosity.Metal nodes and organic linkers form ordered lattices with defined pores,enabling predictable adsorp-tion and transport processes.Traditionally,research on MOFs has primarily focused on established fields such as molecular adsorption and heterogeneous catalysis[1,2]
基金supported by the National Natural Science Foundation of China (U1507116, 21471152, and 21477130)the Major Research Plan of Natural Science Foundation of China (91326202)The Science Challenge Project of China (JCKY2016212A504) is also acknowledged
文摘Here we present a combined DFF and molecular dynamics study of uranyl （U（VI）） interaction mecha- nisms with the calcite （104） surface in aqueous solution. The roles of three anion ligands （CO2 , HCO3, OH ） and solvation effect in U（VI） interaction with calcite have been evaluated. According to our calculations, water adsorbed on the calcite （104） surface prefers to exist in molecular state rather than dis- sociative state. Energy analysis indicate that the positively charged uranyl species prefers to form surface complexes on the surface, while neutral uranyl species may bind with the surface via both surface complexing and ion exchange reactions of U（VI） → Ca（II）. In contrast, the negatively charged uranyl species prefer to interact with the surface via ion exchange reactions of U（VI）→ Ca（II）, and the one with UO2（CO3）2（H2O）^2- as the reactant becomes the most favorable one in energy. We also found that uranyl adsorption increases the hydrophilicability of the （104） surface to different extents, where the UO2（CO3）3Ca2 species contributes to the largest degree of energy changes （ 53 kcal/mol）. Our calcula- tions proved that the （104） surface also has the ability to immobilize U（VI） via either surface complexing or ion exchange mechanisms under different pH values.
基金support by the National University of Singapore start-up grant,Centre for Hydrogen Innovations(grant no.CHI-P2023-04)National Research Foundation of Singapore(grant No.U2411D4005)+2 种基金Ministry of Education(grant no.23-0646-A0001 and T2EP50124-0006)the National Research Foundation(grant no.24-1637-A0004)Prime Minister’s Office,Singapore under its Campus for Research Excellence and Technological Enterprise(CREATE)programme(Development of advanced catalysts for electrochemical carbon abatement).
文摘The pressing challenges of the energy crisis and environmental problems necessitate the pursuit of efficient and sustainable energy conversion technologies,wherein catalytic processes play a vital role in addressing these issues.Single-molecule fluorescence microscopy(SMFM)offers a transformative approach to understanding various catalytic reactions by enabling real-time visualization of molecular adsorption,diffusion,and transformation on catalytic surfaces.The unprecedented insights into the spatial distribution of active sites,catalytic heterogeneity,and the dynamics of key intermediates result in single-or subparticle level structure−property relations,thereby offering insightful perspectives for catalyst design and mechanistic understanding of energy-related catalytic processes.In this review,we provide an overview of the recent progress in using SMFM for investigating energy-related catalytic reactions.The advancement in SMFM imaging techniques for investigating nonfluorescent chemical processes is also highlighted.Finally,we conclude the review by commenting on the current challenges and prospects in advancing SMFM in energy research.We hope that the capable SMFM imaging techniques and insights will promote the development and realistic application of various energy-related catalytic reactions,together with inspiring researchers to explore the power of SMFM in other applications.
