BACKGROUND Many patients with ulcerative colitis(UC)do not respond well to,or tolerate conventional and biological therapies.There is currently no consensus on the treatment of refractory UC.Studies have demonstrated ...BACKGROUND Many patients with ulcerative colitis(UC)do not respond well to,or tolerate conventional and biological therapies.There is currently no consensus on the treatment of refractory UC.Studies have demonstrated that the selective Janus kinase 1 inhibitor upadacitinib,a small-molecule drug,is effective and safe for treating UC.However,no studies have revealed that upadacitinib is effective in treating refractory UC with primary nonresponse to infliximab and vedolizumab.CASE SUMMARY We report the case of a 44-year-old male patient with a chief complaint of bloody diarrhoea with mucus and pus,in addition to dizziness.The patient had recurrent disease after receiving mesalazine,prednisone,azathioprine,infliximab and vedolizumab over four years.Based on the endoscopic findings and pathological biopsy,the patient was diagnosed with refractory UC.In particular,the patient showed primary nonresponse to infliximab and vedolizumab.Based on the patient’s history and recurrent disease,we decided to administer upadacitinib.During hospitalisation,the patient was received upadacitinib under our guidance.Eight weeks after the initiation of upadacitinib treatment,the patient’s symptoms and endoscopic findings improved significantly.No notable adverse reactions have been reported to date.CONCLUSION Our case report suggests that upadacitinib may represent a valuable strategy for treating refractory UC with primary nonresponse.展开更多
Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an u...Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an urgent requirement.In this paper,we successfully synthesized Co_(2)VO_(4)/Co compounds with Co-VMOF(metal-organic framework)as a sacrificial template and investigated their electrochemical mechanism in order to improve the electrochemical properties of LIBs and SIBs.The optimized heaping configuration and the existence of metallic Co catalyzed the formation of radical ions,thereby facilitating higher conductivity,shortening Li+and Na+transport paths,and providing more active sites.Co_(2)VO_(4)/Co constructed with 2-methylimidazole as a ligand showed a discharge capacity of 1605.1 mA h g^(-1)after 300 cycles at 0.1 A g^(-1)in LIB and 677.2 mA h g^(-1)in SIB.Density functional theory(DFT)calculation emphasizes the crucial role of Co_(2)VO_(4)/Co in enhancing electrode conductivity,decreasing the migratory energy barrier,and thereby strengthening electrochemical properties.This heterostructure building technique may pave the way for the development of high-performance LIBs and SIBs.Furthermore,the problem of the low first-loop coulombic efficiency faced by transition metal oxides is improved.展开更多
The balance between cationic redox and oxygen redox in layer-structured cathode materials is an important issue for sodium batteries to obtain high energy density and considerable cycle stability.Oxygen redox can cont...The balance between cationic redox and oxygen redox in layer-structured cathode materials is an important issue for sodium batteries to obtain high energy density and considerable cycle stability.Oxygen redox can contribute extra capacity to increase energy density,but results in lattice instability and capacity fading caused by lattice oxygen gliding and oxygen release.In this work,reversible Mn^(2+)/Mn^(4+)redox is realized in a P3-Na_(0.65)Li_(0.2)Co_(0.05)Mn_(0.75)O_(2)cathode material with high specific capacity and structure stability via Co substitution.The contribution of oxygen redox is suppressed significantly by reversible Mn^(2+)/Mn^(4+)redox without sacrificing capacity,thus reducing lattice oxygen release and improving the structure stability.Synchrotron X-ray techniques reveal that P3 phase is well maintained in a wide voltage window of 1.5-4.5 V vs.Na^(+)/Na even at 10 C and after long-term cycling.It is disclosed that charge compensation from Co/Mn-ions contributes to the voltage region below 4.2 V and O-ions contribute to the whole voltage range.The synergistic contributions of Mn^(2+)/Mn^(4+),Co^(2+)/Co^(3+),and O^(2-)/(O_n)^(2-)redox in P3-Na_(0.65)Li_(0.2)Co_(0.05)Mn_(0.75)O_(2)lead to a high reversible capacity of 215.0 m A h g^(-1)at 0.1 C with considerable cycle stability.The strategy opens up new opportunities for the design of high capacity cathode materials for rechargeable batteries.展开更多
为应对风力机齿轮箱振动信号压缩与重构过程存在复杂的参数设置问题,提出了基于模拟退火多种群遗传算法(Simulating Annealing and Multiple Population Genetic Algorithm,SA-MPGA)自适应设置过完备学习字典生成、振动信号压缩、压缩...为应对风力机齿轮箱振动信号压缩与重构过程存在复杂的参数设置问题,提出了基于模拟退火多种群遗传算法(Simulating Annealing and Multiple Population Genetic Algorithm,SA-MPGA)自适应设置过完备学习字典生成、振动信号压缩、压缩信号重构过程所需参数集。在传统遗传算法基础上引入多种群思想,增加了遗传算法对解空间的覆盖。在种群繁衍时个体选择引入模拟退火策略在种群进化过程中以不同概率接受一定程度的劣解,从而有助于遗传算法跳出局部最优解的缺陷。基于SA-MPGA的多参数自适应选择降低了传统遗传算法容易收敛到局部最优解的概率。应用实际工程数据验证基于SA-MPGA多参数优化问题,实验结果表明,在保持压缩率的前提下,基于模拟退火多种群算法比基于遗传算法重构信号与原始信号的峰值信噪比提升了16.5%,相关性提升了12.5%,均方根误差降低了13.4%。展开更多
Hyperhomocysteinemia and abnormal blood lipids are independent risk factors for stroke. However, whether both factors exert a synergistic effect in the onset of stroke remains unclear. The present study is a retrospec...Hyperhomocysteinemia and abnormal blood lipids are independent risk factors for stroke. However, whether both factors exert a synergistic effect in the onset of stroke remains unclear. The present study is a retrospective analysJs of 2 089 cases of stroke and 2 089 control cases of simple in- tervertebral disk protrusion using a paired multivariate logistic regression method. Adjusting for known confounding variables including the patients＇ age, gender, smoking status, alcohol con- sumption status, patient and family medical history, and clinical biochemical indices, elevated ho- mocysteine level was related to the onset of stroke. Patients with elevated homocysteJne levels and abnormal blood lipids showed a 40.9 % increase in the risk for stroke compared to patients with normal homocysteine levels and blood lipids （odds ratio 1.409; 95% confidence interval 1.127-1.761）. These results indicate that elevated homocysteine and abnormal blood lipids exert synergistic effects in the onset of stroke. Patients with elevated homocysteine levels and abnormal blood lipids are predisposed to stroke.展开更多
Development of highly active and stable non-noble electrocatalysts with well-defined nanostructures is crucial for efficient hydrogen evolution reaction(HER). Herein, a novel three-dimensional(3D) selfsupported electr...Development of highly active and stable non-noble electrocatalysts with well-defined nanostructures is crucial for efficient hydrogen evolution reaction(HER). Herein, a novel three-dimensional(3D) selfsupported electrode consists of vanadium nitride(VN) nanodots and Co nanoparticles co-embedded and highly active single Co atoms anchored in N-doped carbon nanotubes supported on carbon cloth(VN-Co@CoSAs-NCNTs/CC) is fabricated via a one-step in situ nanoconfined pyrolysis strategy, which shows remarkable enhanced HER electrocatalytic activity in acidic medium. During pyrolysis, the formed VN nanodots induce the generation of atomic Co Nxsites in NCNTs, contributing to superior electrocatalytic activity. Experimental and density functional theory(DFT) calculation results reveal that the electrode has multiple accessible active sites, fast reaction kinetics, low charge/mass transfer resistances,high conductivity, as well as downshifted d-band center with a thermodynamically favorable hydrogen adsorption free energy(△G_(H·)), all of which greatly boost the HER performance. As a result, the VNCo@CoSAs-NCNTs/CC electrode displays superb catalytic performance toward HER with a low overpotential of 29 mV at 10 mA cm^(-2) in acidic medium, which could maintain for at least 60 h of stable performance. This work opens a facile avenue to explore low-cost, high performance, but inexpensive metals/nitrogen-doped carbon composite electrocatalysts for HER.展开更多
The electrochemical reduction of nitrate to ammonia(NH3) can be used to recycle nitrogen and offers a decarbonized route for sustainable NH3production,but requires efficient electrocatalysts.Herein,we have rationally ...The electrochemical reduction of nitrate to ammonia(NH3) can be used to recycle nitrogen and offers a decarbonized route for sustainable NH3production,but requires efficient electrocatalysts.Herein,we have rationally designed and fabricated a novel self-supported electrocatalyst comprised of Ni nanoparticles(NiNPs) embedded in Ni single atoms(NiSAs) anchored to nitrogen-doped carbon nanotubes grown on carbon cloth(NiNPs@NiSAs-NCNTs/CC) used for an efficient nitrate reduction reaction(NO3-RR) to produce NH_(3).The electrocatalyst can attain a maximum NH3yield rate of 27.67±1.16 mgNH3h^(-1)cm^(-2)at-1.4 V vs.reversible hydrogen electrode(RHE) and nearly 100% Faradic efficiency in the range of-1.2--1.4 V vs.RHE in a neutral medium,outperforming the previously reported Ni-based catalysts.Our experimental analysis and theoretical calculations have demonstrated that the moderate electrondeficient state of NiSAsregulated by NiNPsnot only facilitates the enrichment of NO_(3)^(-),but also benefits the formation of NO3*and decrease in the energy barrier of the rate-limiting step,thus resulting in the enhanced NO3-RR performance.展开更多
In order to quantitate the bovine immunodeficiency virus line （BIVL） was established by transfecting baby hamster kidney （BIV） cells infection in vitro, a BIV indicator cell with reporter plasmids containing the f...In order to quantitate the bovine immunodeficiency virus line （BIVL） was established by transfecting baby hamster kidney （BIV） cells infection in vitro, a BIV indicator cell with reporter plasmids containing the firefly luciferase gene driven by a BIV long terminal repeat promoter. The BIV activates promoter activity of the LTR to express luciferase upon infection. BIV infection could therefore by quantified by detection of luciferase activity. Compared to standard assays used to detect BIV infection, the BIVL-based assay is 10 times more sensitive than the the CPE-based assay, and has similar sensitivity with the viral capsid protein Western blot assay BIV indicator cell line could detect BIV infection specifically. Luciferase activity of BIV infected BIVL cells showed a time dependent manner, and 60 h post infection is the optimal time to detect BIV infection. Luciferase activity of BIVL cells correlates with the BIV capsid protein expression. Moreover, a linear relationship was found between MOI and the activated intensity of luciferase expression. In brief, the BIV indicator cell line is an easy, robust and quantitive method for monitoring BIV infection.展开更多
To study the Fe-M interactions and their effects on 31p NMR, the structures of Fe（CO）3（EtPhPpy）2 1, Fe（CO）3（EtPhPpy）2M（NCS）2 （2： M=Zn, 3： M=Cd, 4： M=Hg） and Fe（CO）3（EtPhPpy）2CdX2 （5： X=C1, 6： X=...To study the Fe-M interactions and their effects on 31p NMR, the structures of Fe（CO）3（EtPhPpy）2 1, Fe（CO）3（EtPhPpy）2M（NCS）2 （2： M=Zn, 3： M=Cd, 4： M=Hg） and Fe（CO）3（EtPhPpy）2CdX2 （5： X=C1, 6： X=SCN） were investigated by density functional theory （DFT） PBE0 method. The stabilities S of complexes follow S（2）〉S（3）〉S（4） and S（3）,.~S（6）〉S（5）, indicating that 6 is stable and may be synthesized. The complexes with thiocyanate are more stable than that with chloride in Fe（CO）3（EtPhPpy）2CdX2. The strength I of Fe-M interactions follows I（2）≈I（3）〈I（4）. The Fe-Cd interactions of 3 and 6, which contain thiocyanate, are stronger than that of 5 with chloride. The charge-transfer, which enhances with the increasing of Fe-M interaction strength, comes from Et, Ph, py, CO groups towards P, Fe, and M atoms. Because the delocalization of thiocyanate disperses the charge of M2＋, the charge-transfer of the complexes with thiocyanate is stronger than that with chloride. There is a a-bond between Fe and Hg atoms in 4. However, in binuclear complexes except 4, the Fe-M interactions act as nFe→nM, σP-Fe→nM and σC-Fe→nM delocalization, and the N-M interactions mainly act as nN→nM delocalization. In binuclear complexes, due to the Fe→M interactions, the strong σFe--C→σ＊Fe--p or σFe-Hg→σ＊Fe--I2 delocalization and the charge-transfer, the electron density on P nucleus is increased, and thus upfield 31p chemical shifts are caused （compared with mononuclear complex 1）.展开更多
Metal-organic frameworks(MOFs)can serve as prevailing anodes for lithium-ion batteries,due to their multiple redox-active sites and prominent structural compatibility.However,the poor electronic conductivity and infer...Metal-organic frameworks(MOFs)can serve as prevailing anodes for lithium-ion batteries,due to their multiple redox-active sites and prominent structural compatibility.However,the poor electronic conductivity and inferior cyclability hinder their further implementation.Herein,a synthetic methodology for trimetallic Fe-Co-Ni MOFs with nanoframe superstructures architecture(Fe-Co-Ni NFSs)via structural evolution is proposed for versatile anode materials for lithium storage.Ascribed to optimal compositional and structural optimization,the Fe-Co-Ni NFSs achieve exceptional electrochemical performance with superior specific capacity(1030 mAh g^(−1) at 0.1 A g^(−1)),outstanding rate capacity(414 mAh g^(−1) at 2 A g^(−1)),and prolonged cyclability(489 mAh g^(−1) upon 1000 cycles at 1 A g^(−1)).Both experimental and theoretical investigations reveal that the multi-component metal centers could boost electronic conductivity,confer multiple active sites,and energetically favor Li adsorption capability.Additionally,the nanoframe superstructures of Fe-Co-Ni NFSs could facilitate stress-buffering effect on volumetric expansion and prevent electrode pulverization,further improving the lithium storage capability.This work envisions a meticulous protocol for high-performance MOF anode materials for lithium-ion batteries.展开更多
Three polyoxometalate-based hybrid coordination materials,[Co_(8)(H_(2)O)_(34)(pz)_(2){Co_(4)(H_(2)O)_(2)P_(4)W_(30)O_(112)}]·16H_(2)O(compound 1),[H_(3)O]_(4)[Co_(6)(H_(2)O)_(22)(pz)_(2){Co_(4)(H_(2)O)_(2)P_(4)W...Three polyoxometalate-based hybrid coordination materials,[Co_(8)(H_(2)O)_(34)(pz)_(2){Co_(4)(H_(2)O)_(2)P_(4)W_(30)O_(112)}]·16H_(2)O(compound 1),[H_(3)O]_(4)[Co_(6)(H_(2)O)_(22)(pz)_(2){Co_(4)(H_(2)O)_(2)P_(4)W_(30)O_(112)}]·21H_(2)(compound 2),and[H_(3)O]_(4)[Co_(6)(H_(2)O)_(22){Co_(4)(H_(2)O)_(2)P_(4)W_(30)O_(112)}]·29H_(2)O(compound 3)(pz-pyrazine),were built from the linkage of[Co_(4)(H_(2)O)_(2)(P_(2)W_(15)O_(56)_(2)]^(16-)-(abbreviated as{Co_(4)P_(4)W_(30})polyanions and pz and/or cobalt(II)cations.Although compounds 1 and 2 consisted of the same components,their lamellar networks were quite different.The inorganic lamellar network in compound 3 was constructed by connecting{Co_(4)P_(4)W_(30)}units with cobalt(I)cations.This work demonstrates that the coordination modes of{Co_(4)P_(4)W_(30)}are very sensitive to synthesis conditions,while the ring-belt tetrametals are easily substituted by different transition metal cations under mild reaction conditions.展开更多
A novel coupled system using Co–Ti O2 was successfully designed which combined two different heterogeneous advanced oxidation processes, sulfate radical based Fenton-like reaction（SR-Fenton） and visible light photo...A novel coupled system using Co–Ti O2 was successfully designed which combined two different heterogeneous advanced oxidation processes, sulfate radical based Fenton-like reaction（SR-Fenton） and visible light photocatalysis（Vis-Photo）, for degradation of organic contaminants. The synergistic effect of SR-Fenton and Vis-Photo was observed through comparative tests of 50 mg/L Rhodamine B（Rh B） degradation and TOC removal. The Rhodamine B degradation rate and TOC removal were 100% and 68.1% using the SR-Fenton/Vis-Photo combined process under ambient conditions, respectively. Moreover, based on XRD, XPS and UV-DRS characterization, it can be deduced that tricobalt tetroxide located on the surface of the catalyst is the SR-Fenton active site, and cobalt ion implanted in the Ti O2 lattice is the reason for the visible light photocatalytic activity of Co–Ti O2. Finally, the effects of the calcination temperature and cobalt concentration on the synergistic performance were also investigated and a possible mechanism for the synergistic system was proposed. This coupled system exhibited excellent catalytic stability and reusability,and almost no dissolution of Co2＋was found.展开更多
Focal epilepsy accounts for 60% of all forms of epilepsy, but the pathogenic mechanism is not well understood. In this study,three novel mutations in NPRL3(nitrogen permease regulator-like 3), c.937_945del, c.1514dup ...Focal epilepsy accounts for 60% of all forms of epilepsy, but the pathogenic mechanism is not well understood. In this study,three novel mutations in NPRL3(nitrogen permease regulator-like 3), c.937_945del, c.1514dup C and 6,706-bp genomic DNA(g DNA) deletion, were identified in three families with focal epilepsy by linkage analysis, whole exome sequencing(WES) and Sanger sequencing. NPRL3 protein is a component of the GATOR1 complex, a major inhibitor of m TOR signaling. These mutations led to truncation of the NPRL3 protein and hampered the binding between NPRL3 and DEPDC5, which is another component of the GATOR1 complex. Consequently, the mutant proteins enhanced m TOR signaling in cultured cells, possibly due to impaired inhibition of m TORC1 by GATOR1. Knockdown of nprl3 in Drosophila resulted in epilepsy-like behavior and abnormal synaptic development. Taken together, these findings expand the genotypic spectrum of NPRL3-associated focal epilepsy and provide further insight into how NPRL3 mutations lead to epilepsy.展开更多
基金Supported by Shenzhen Science and Technology Program,No.JCYJ20220530154013031Guangdong Province Health and Health Appropriate Technology Promotion Project,No.2023385Guangdong Province Grassroots Science Popularization Action Plan,No.20240205.
文摘BACKGROUND Many patients with ulcerative colitis(UC)do not respond well to,or tolerate conventional and biological therapies.There is currently no consensus on the treatment of refractory UC.Studies have demonstrated that the selective Janus kinase 1 inhibitor upadacitinib,a small-molecule drug,is effective and safe for treating UC.However,no studies have revealed that upadacitinib is effective in treating refractory UC with primary nonresponse to infliximab and vedolizumab.CASE SUMMARY We report the case of a 44-year-old male patient with a chief complaint of bloody diarrhoea with mucus and pus,in addition to dizziness.The patient had recurrent disease after receiving mesalazine,prednisone,azathioprine,infliximab and vedolizumab over four years.Based on the endoscopic findings and pathological biopsy,the patient was diagnosed with refractory UC.In particular,the patient showed primary nonresponse to infliximab and vedolizumab.Based on the patient’s history and recurrent disease,we decided to administer upadacitinib.During hospitalisation,the patient was received upadacitinib under our guidance.Eight weeks after the initiation of upadacitinib treatment,the patient’s symptoms and endoscopic findings improved significantly.No notable adverse reactions have been reported to date.CONCLUSION Our case report suggests that upadacitinib may represent a valuable strategy for treating refractory UC with primary nonresponse.
基金financially supported by the Open Fund of Energy and Materials Chemistry Joint Laboratory of SCNU and TINCI,China (SCNU-TINCI-202207)。
文摘Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an urgent requirement.In this paper,we successfully synthesized Co_(2)VO_(4)/Co compounds with Co-VMOF(metal-organic framework)as a sacrificial template and investigated their electrochemical mechanism in order to improve the electrochemical properties of LIBs and SIBs.The optimized heaping configuration and the existence of metallic Co catalyzed the formation of radical ions,thereby facilitating higher conductivity,shortening Li+and Na+transport paths,and providing more active sites.Co_(2)VO_(4)/Co constructed with 2-methylimidazole as a ligand showed a discharge capacity of 1605.1 mA h g^(-1)after 300 cycles at 0.1 A g^(-1)in LIB and 677.2 mA h g^(-1)in SIB.Density functional theory(DFT)calculation emphasizes the crucial role of Co_(2)VO_(4)/Co in enhancing electrode conductivity,decreasing the migratory energy barrier,and thereby strengthening electrochemical properties.This heterostructure building technique may pave the way for the development of high-performance LIBs and SIBs.Furthermore,the problem of the low first-loop coulombic efficiency faced by transition metal oxides is improved.
基金financially supported by the National Key Scientific Research Project(2022YFB2502300)China and the National Natural Science Foundation of China(52071085)。
文摘The balance between cationic redox and oxygen redox in layer-structured cathode materials is an important issue for sodium batteries to obtain high energy density and considerable cycle stability.Oxygen redox can contribute extra capacity to increase energy density,but results in lattice instability and capacity fading caused by lattice oxygen gliding and oxygen release.In this work,reversible Mn^(2+)/Mn^(4+)redox is realized in a P3-Na_(0.65)Li_(0.2)Co_(0.05)Mn_(0.75)O_(2)cathode material with high specific capacity and structure stability via Co substitution.The contribution of oxygen redox is suppressed significantly by reversible Mn^(2+)/Mn^(4+)redox without sacrificing capacity,thus reducing lattice oxygen release and improving the structure stability.Synchrotron X-ray techniques reveal that P3 phase is well maintained in a wide voltage window of 1.5-4.5 V vs.Na^(+)/Na even at 10 C and after long-term cycling.It is disclosed that charge compensation from Co/Mn-ions contributes to the voltage region below 4.2 V and O-ions contribute to the whole voltage range.The synergistic contributions of Mn^(2+)/Mn^(4+),Co^(2+)/Co^(3+),and O^(2-)/(O_n)^(2-)redox in P3-Na_(0.65)Li_(0.2)Co_(0.05)Mn_(0.75)O_(2)lead to a high reversible capacity of 215.0 m A h g^(-1)at 0.1 C with considerable cycle stability.The strategy opens up new opportunities for the design of high capacity cathode materials for rechargeable batteries.
文摘为应对风力机齿轮箱振动信号压缩与重构过程存在复杂的参数设置问题,提出了基于模拟退火多种群遗传算法(Simulating Annealing and Multiple Population Genetic Algorithm,SA-MPGA)自适应设置过完备学习字典生成、振动信号压缩、压缩信号重构过程所需参数集。在传统遗传算法基础上引入多种群思想,增加了遗传算法对解空间的覆盖。在种群繁衍时个体选择引入模拟退火策略在种群进化过程中以不同概率接受一定程度的劣解,从而有助于遗传算法跳出局部最优解的缺陷。基于SA-MPGA的多参数自适应选择降低了传统遗传算法容易收敛到局部最优解的概率。应用实际工程数据验证基于SA-MPGA多参数优化问题,实验结果表明,在保持压缩率的前提下,基于模拟退火多种群算法比基于遗传算法重构信号与原始信号的峰值信噪比提升了16.5%,相关性提升了12.5%,均方根误差降低了13.4%。
基金supported by a grant from Medical Science DataSharing Network,Ministry of Science and Technology,China,No.2005DKA32403Military Medical Scientific Research grants,No.11BJZ32,No.12BJZ271 and No.10BJZ202
文摘Hyperhomocysteinemia and abnormal blood lipids are independent risk factors for stroke. However, whether both factors exert a synergistic effect in the onset of stroke remains unclear. The present study is a retrospective analysJs of 2 089 cases of stroke and 2 089 control cases of simple in- tervertebral disk protrusion using a paired multivariate logistic regression method. Adjusting for known confounding variables including the patients＇ age, gender, smoking status, alcohol con- sumption status, patient and family medical history, and clinical biochemical indices, elevated ho- mocysteine level was related to the onset of stroke. Patients with elevated homocysteJne levels and abnormal blood lipids showed a 40.9 % increase in the risk for stroke compared to patients with normal homocysteine levels and blood lipids （odds ratio 1.409; 95% confidence interval 1.127-1.761）. These results indicate that elevated homocysteine and abnormal blood lipids exert synergistic effects in the onset of stroke. Patients with elevated homocysteine levels and abnormal blood lipids are predisposed to stroke.
基金supported by grants from the National Natural Science Foundation of China (21971129, 21961022, 21661023,21802076, and 21962013)the 111 Project (D20033)+2 种基金the Natural Science Foundation of Inner Mongolia Autonomous Region of China (2018BS05007)the Program of Higher-level Talents of IMU (21300-5195109)the Cooperation Project of State Key Laboratory of Baiyun Obo Rare Earth Resource Researches and Comprehensive Utilization (2017Z1950)。
文摘Development of highly active and stable non-noble electrocatalysts with well-defined nanostructures is crucial for efficient hydrogen evolution reaction(HER). Herein, a novel three-dimensional(3D) selfsupported electrode consists of vanadium nitride(VN) nanodots and Co nanoparticles co-embedded and highly active single Co atoms anchored in N-doped carbon nanotubes supported on carbon cloth(VN-Co@CoSAs-NCNTs/CC) is fabricated via a one-step in situ nanoconfined pyrolysis strategy, which shows remarkable enhanced HER electrocatalytic activity in acidic medium. During pyrolysis, the formed VN nanodots induce the generation of atomic Co Nxsites in NCNTs, contributing to superior electrocatalytic activity. Experimental and density functional theory(DFT) calculation results reveal that the electrode has multiple accessible active sites, fast reaction kinetics, low charge/mass transfer resistances,high conductivity, as well as downshifted d-band center with a thermodynamically favorable hydrogen adsorption free energy(△G_(H·)), all of which greatly boost the HER performance. As a result, the VNCo@CoSAs-NCNTs/CC electrode displays superb catalytic performance toward HER with a low overpotential of 29 mV at 10 mA cm^(-2) in acidic medium, which could maintain for at least 60 h of stable performance. This work opens a facile avenue to explore low-cost, high performance, but inexpensive metals/nitrogen-doped carbon composite electrocatalysts for HER.
基金supported by the National Natural Science Foundation of China(21971129, 21961022, 21661023, 22172083, and 21962013)the Inner Mongolia Autonomous Region 2022 Leading Talent Team of Science and Technology (2022LJRC0008)+8 种基金the Natural Science Foundation of Inner Mongolia Autonomous Region of China(2022BS02014 and 2021BS02007)the 111 Project (D20033)the Natural Science Foundation of Inner Mongolia Autonomous Region of China (2021JQ02)the Program for Innovative Research Team in Universities of Inner Mongolia Autonomous Region (NJYT23031)the Program of Higher-level Talents of IMU (21300-5215101)the“Grassland Leading Talent” Program of Inner Mongoliathe“Grassland Talent” Innovation Team of Inner Mongoliathe“Science and Technology for a Better Development of Inner Mongolia” Program(2020XM03)the Science and Technology Project of Ordos(2021 ZDI 11-14)。
文摘The electrochemical reduction of nitrate to ammonia(NH3) can be used to recycle nitrogen and offers a decarbonized route for sustainable NH3production,but requires efficient electrocatalysts.Herein,we have rationally designed and fabricated a novel self-supported electrocatalyst comprised of Ni nanoparticles(NiNPs) embedded in Ni single atoms(NiSAs) anchored to nitrogen-doped carbon nanotubes grown on carbon cloth(NiNPs@NiSAs-NCNTs/CC) used for an efficient nitrate reduction reaction(NO3-RR) to produce NH_(3).The electrocatalyst can attain a maximum NH3yield rate of 27.67±1.16 mgNH3h^(-1)cm^(-2)at-1.4 V vs.reversible hydrogen electrode(RHE) and nearly 100% Faradic efficiency in the range of-1.2--1.4 V vs.RHE in a neutral medium,outperforming the previously reported Ni-based catalysts.Our experimental analysis and theoretical calculations have demonstrated that the moderate electrondeficient state of NiSAsregulated by NiNPsnot only facilitates the enrichment of NO_(3)^(-),but also benefits the formation of NO3*and decrease in the energy barrier of the rate-limiting step,thus resulting in the enhanced NO3-RR performance.
基金The General Foundation of Tianjin Science Committee for Applied Basic Research (08JCZDJC21000)Chinese Ministry of Education (30770081)
文摘In order to quantitate the bovine immunodeficiency virus line （BIVL） was established by transfecting baby hamster kidney （BIV） cells infection in vitro, a BIV indicator cell with reporter plasmids containing the firefly luciferase gene driven by a BIV long terminal repeat promoter. The BIV activates promoter activity of the LTR to express luciferase upon infection. BIV infection could therefore by quantified by detection of luciferase activity. Compared to standard assays used to detect BIV infection, the BIVL-based assay is 10 times more sensitive than the the CPE-based assay, and has similar sensitivity with the viral capsid protein Western blot assay BIV indicator cell line could detect BIV infection specifically. Luciferase activity of BIV infected BIVL cells showed a time dependent manner, and 60 h post infection is the optimal time to detect BIV infection. Luciferase activity of BIVL cells correlates with the BIV capsid protein expression. Moreover, a linear relationship was found between MOI and the activated intensity of luciferase expression. In brief, the BIV indicator cell line is an easy, robust and quantitive method for monitoring BIV infection.
基金This work was supported by the Natural Science Foundation of Guangdong Province （No.5005938） and the Research Project of Ministry of Education and Guangdong Province （No.2007A090302046）.
文摘To study the Fe-M interactions and their effects on 31p NMR, the structures of Fe（CO）3（EtPhPpy）2 1, Fe（CO）3（EtPhPpy）2M（NCS）2 （2： M=Zn, 3： M=Cd, 4： M=Hg） and Fe（CO）3（EtPhPpy）2CdX2 （5： X=C1, 6： X=SCN） were investigated by density functional theory （DFT） PBE0 method. The stabilities S of complexes follow S（2）〉S（3）〉S（4） and S（3）,.~S（6）〉S（5）, indicating that 6 is stable and may be synthesized. The complexes with thiocyanate are more stable than that with chloride in Fe（CO）3（EtPhPpy）2CdX2. The strength I of Fe-M interactions follows I（2）≈I（3）〈I（4）. The Fe-Cd interactions of 3 and 6, which contain thiocyanate, are stronger than that of 5 with chloride. The charge-transfer, which enhances with the increasing of Fe-M interaction strength, comes from Et, Ph, py, CO groups towards P, Fe, and M atoms. Because the delocalization of thiocyanate disperses the charge of M2＋, the charge-transfer of the complexes with thiocyanate is stronger than that with chloride. There is a a-bond between Fe and Hg atoms in 4. However, in binuclear complexes except 4, the Fe-M interactions act as nFe→nM, σP-Fe→nM and σC-Fe→nM delocalization, and the N-M interactions mainly act as nN→nM delocalization. In binuclear complexes, due to the Fe→M interactions, the strong σFe--C→σ＊Fe--p or σFe-Hg→σ＊Fe--I2 delocalization and the charge-transfer, the electron density on P nucleus is increased, and thus upfield 31p chemical shifts are caused （compared with mononuclear complex 1）.
基金We gratefully acknowledge the financial support from the Guangzhou Science and Technology Project (No.201904010213).
文摘Metal-organic frameworks(MOFs)can serve as prevailing anodes for lithium-ion batteries,due to their multiple redox-active sites and prominent structural compatibility.However,the poor electronic conductivity and inferior cyclability hinder their further implementation.Herein,a synthetic methodology for trimetallic Fe-Co-Ni MOFs with nanoframe superstructures architecture(Fe-Co-Ni NFSs)via structural evolution is proposed for versatile anode materials for lithium storage.Ascribed to optimal compositional and structural optimization,the Fe-Co-Ni NFSs achieve exceptional electrochemical performance with superior specific capacity(1030 mAh g^(−1) at 0.1 A g^(−1)),outstanding rate capacity(414 mAh g^(−1) at 2 A g^(−1)),and prolonged cyclability(489 mAh g^(−1) upon 1000 cycles at 1 A g^(−1)).Both experimental and theoretical investigations reveal that the multi-component metal centers could boost electronic conductivity,confer multiple active sites,and energetically favor Li adsorption capability.Additionally,the nanoframe superstructures of Fe-Co-Ni NFSs could facilitate stress-buffering effect on volumetric expansion and prevent electrode pulverization,further improving the lithium storage capability.This work envisions a meticulous protocol for high-performance MOF anode materials for lithium-ion batteries.
基金This work is supported by the National Natural Science Foundation of China(Nos.21525312 and 21872122).
文摘Three polyoxometalate-based hybrid coordination materials,[Co_(8)(H_(2)O)_(34)(pz)_(2){Co_(4)(H_(2)O)_(2)P_(4)W_(30)O_(112)}]·16H_(2)O(compound 1),[H_(3)O]_(4)[Co_(6)(H_(2)O)_(22)(pz)_(2){Co_(4)(H_(2)O)_(2)P_(4)W_(30)O_(112)}]·21H_(2)(compound 2),and[H_(3)O]_(4)[Co_(6)(H_(2)O)_(22){Co_(4)(H_(2)O)_(2)P_(4)W_(30)O_(112)}]·29H_(2)O(compound 3)(pz-pyrazine),were built from the linkage of[Co_(4)(H_(2)O)_(2)(P_(2)W_(15)O_(56)_(2)]^(16-)-(abbreviated as{Co_(4)P_(4)W_(30})polyanions and pz and/or cobalt(II)cations.Although compounds 1 and 2 consisted of the same components,their lamellar networks were quite different.The inorganic lamellar network in compound 3 was constructed by connecting{Co_(4)P_(4)W_(30)}units with cobalt(I)cations.This work demonstrates that the coordination modes of{Co_(4)P_(4)W_(30)}are very sensitive to synthesis conditions,while the ring-belt tetrametals are easily substituted by different transition metal cations under mild reaction conditions.
基金supported by the Fundamental Research Funds for the Central Universities(No.CDJXS12210002)the Major Project Foundation of Science and Technology Innovation in Minister of Education(No.708071)+2 种基金the Financial Supports of the National Natural Science Foundation of China(No.51108483)Natural Science Foundation Project of CQ CSTC(No.cstcjjA 20002)the 111 Project(No.B13041)
文摘A novel coupled system using Co–Ti O2 was successfully designed which combined two different heterogeneous advanced oxidation processes, sulfate radical based Fenton-like reaction（SR-Fenton） and visible light photocatalysis（Vis-Photo）, for degradation of organic contaminants. The synergistic effect of SR-Fenton and Vis-Photo was observed through comparative tests of 50 mg/L Rhodamine B（Rh B） degradation and TOC removal. The Rhodamine B degradation rate and TOC removal were 100% and 68.1% using the SR-Fenton/Vis-Photo combined process under ambient conditions, respectively. Moreover, based on XRD, XPS and UV-DRS characterization, it can be deduced that tricobalt tetroxide located on the surface of the catalyst is the SR-Fenton active site, and cobalt ion implanted in the Ti O2 lattice is the reason for the visible light photocatalytic activity of Co–Ti O2. Finally, the effects of the calcination temperature and cobalt concentration on the synergistic performance were also investigated and a possible mechanism for the synergistic system was proposed. This coupled system exhibited excellent catalytic stability and reusability,and almost no dissolution of Co2＋was found.
基金supported by the National Natural Science Foundation of China (32270663, 31871262, U20A20355,32022035)Shanghai Municipal Science and Technology Major Project(2018SHZDZX05)the Ministry of Science and Technology of China STI2030-Major Projects (2021ZD0203202)。
文摘Focal epilepsy accounts for 60% of all forms of epilepsy, but the pathogenic mechanism is not well understood. In this study,three novel mutations in NPRL3(nitrogen permease regulator-like 3), c.937_945del, c.1514dup C and 6,706-bp genomic DNA(g DNA) deletion, were identified in three families with focal epilepsy by linkage analysis, whole exome sequencing(WES) and Sanger sequencing. NPRL3 protein is a component of the GATOR1 complex, a major inhibitor of m TOR signaling. These mutations led to truncation of the NPRL3 protein and hampered the binding between NPRL3 and DEPDC5, which is another component of the GATOR1 complex. Consequently, the mutant proteins enhanced m TOR signaling in cultured cells, possibly due to impaired inhibition of m TORC1 by GATOR1. Knockdown of nprl3 in Drosophila resulted in epilepsy-like behavior and abnormal synaptic development. Taken together, these findings expand the genotypic spectrum of NPRL3-associated focal epilepsy and provide further insight into how NPRL3 mutations lead to epilepsy.
