Bridging laboratory research and practical utilization is of crucial importance for the development of green ammonia synthetic technologies. A decentralized photo-assisted electrochemical-based demonstrator has been p...Bridging laboratory research and practical utilization is of crucial importance for the development of green ammonia synthetic technologies. A decentralized photo-assisted electrochemical-based demonstrator has been proposed for green ammonia synthesis from renewable electricity, air and water, where well-known defect-laden WO_(3) is used as the working electrode, and a commercially available PV panel supplies renewable electricity. In this demonstrator, defect-laden WO_(3) exhibits the optimum electrochemical NH_(3) formation rate(4.51 × 10^(-12)mol s^(-1)cm^(-2)) in 0.1 M K_(2)SO_(4)in a photovoltaic electrochemical(PV-EC) system. A system-level energy and cost analysis was conducted to investigate its economic viability and a general evaluation tool for system performance and cost estimation was proposed. This advance enables the possibility of integrating the small-scale green ammonia demonstrator into a stand-alone farm system.展开更多
Identification of components and metabolites of traditional Chinese medicines(TCMs)employing liquid chromatography-quadrupole time-of-flight mass spectrometry(LC-Q-TOF MS)techniques with information-dependent acquisit...Identification of components and metabolites of traditional Chinese medicines(TCMs)employing liquid chromatography-quadrupole time-of-flight mass spectrometry(LC-Q-TOF MS)techniques with information-dependent acquisition(IDA)approaches is increasingly frequent.A current drawback of IDA-MS is that the complexity of a sample might prevent important compounds from being triggered in IDA settings.Sequential window acquisition of all theoretical fragment-ion spectra(SWATH)is a dataindependent acquisition(DIA)method where the instrument deterministically fragments all precursor ions within the predefined m/z range in a systematic and unbiased fashion.Herein,the superiority of SWATH on the detection of TCMs’components was firstly investigated by comparing the detection efficiency of SWATH-MS and IDA-MS data acquisition modes,and sanguisorbin extract was used as a mode TCM.After optimizing the setting parameters of SWATH,rolling collision energy(CE)and variable Q1 isolation windows were found to be more efficient for sanguisorbin identification than the fixed CE and fixed Q1 isolation window.More importantly,the qualitative efficiency of SWATH-MS on sanguisorbins was found significantly higher than that of IDA-MS data acquisition.In IDA mode,18 kinds of sanguisorbins were detected in sanguisorbin extract.A total of 47 sanguisorbins were detected when SWATH-MS was used under rolling CE and flexible Q1 isolation window modes.Besides,26 metabolites of sanguisorbins were identified in rat plasma,and their metabolic pathways could be deduced as decarbonylation,oxidization,reduction,methylation,and glucuronidation according to their fragmental ions acquired in SWATH-MS mode.Thus,SWATH-MS data acquisition could provide more comprehensive information for the component and metabolite identification for TCMs than IDA-MS.展开更多
The global antibiotic resistance crisis necessitates urgent solutions.One innovative approach involves potentiating antibiotics and non-antibiotic drugs with adjuvants or boosters.A major drawback of these membrane-ac...The global antibiotic resistance crisis necessitates urgent solutions.One innovative approach involves potentiating antibiotics and non-antibiotic drugs with adjuvants or boosters.A major drawback of these membrane-active boosters is their limited biocompatibility,as they struggle to differentiate between prokaryotic and eukaryotic membranes.This study reports the chemical biology investigation of a dual-action oligoamidine(OA1)booster with a glutathione-triggered decomposition mechanism.OA1,when combined with other antimicrobial molecules,exhibits a triple-targeting mechanism including cell membrane disruption,DNA targeting,and intracellular enzyme inhibition.This multi-targeting mechanism not only enhances the in vitro and in vivo eradication of antibiotic-resistant“ESKAPE”pathogens,but also suppresses the development of bacterial resistance.Furthermore,OA1 maintains its activity in bacterial cells by creating an oxidative environment,while it quickly decomposes in mammalian cells due to high glutathione levels.These mechanistic insights and design principles may provide a feasible approach to develop novel antimicrobial agents and effective anti-resistance combination therapies.展开更多
基金grateful to the Natural Sciences and Engineering Council of Canada for supportthe Nation Natural Science Foundation of China (NSFC 21878162,21872102)+4 种基金support of the NSFC(52102311)the Program for Guangdong Introducing Innovative and Entrepreneurial Teams (2019ZT08L101)the Special Fund for the Sci-tech Innovation Strategy of Guangdong Province(210629095860472)the Shenzhen Natural Science Foundation(GXWD20201231105722002-20200824163747001)the Shenzhen Key Laboratory of Eco-materials and Renewable Energy(ZDSYS20200922160400001)。
文摘Bridging laboratory research and practical utilization is of crucial importance for the development of green ammonia synthetic technologies. A decentralized photo-assisted electrochemical-based demonstrator has been proposed for green ammonia synthesis from renewable electricity, air and water, where well-known defect-laden WO_(3) is used as the working electrode, and a commercially available PV panel supplies renewable electricity. In this demonstrator, defect-laden WO_(3) exhibits the optimum electrochemical NH_(3) formation rate(4.51 × 10^(-12)mol s^(-1)cm^(-2)) in 0.1 M K_(2)SO_(4)in a photovoltaic electrochemical(PV-EC) system. A system-level energy and cost analysis was conducted to investigate its economic viability and a general evaluation tool for system performance and cost estimation was proposed. This advance enables the possibility of integrating the small-scale green ammonia demonstrator into a stand-alone farm system.
基金the National Natural Science Foundation of China(81573559,81530098)the Ministry of National Science and Technique(Grant No.2017ZX09309027)。
文摘Identification of components and metabolites of traditional Chinese medicines(TCMs)employing liquid chromatography-quadrupole time-of-flight mass spectrometry(LC-Q-TOF MS)techniques with information-dependent acquisition(IDA)approaches is increasingly frequent.A current drawback of IDA-MS is that the complexity of a sample might prevent important compounds from being triggered in IDA settings.Sequential window acquisition of all theoretical fragment-ion spectra(SWATH)is a dataindependent acquisition(DIA)method where the instrument deterministically fragments all precursor ions within the predefined m/z range in a systematic and unbiased fashion.Herein,the superiority of SWATH on the detection of TCMs’components was firstly investigated by comparing the detection efficiency of SWATH-MS and IDA-MS data acquisition modes,and sanguisorbin extract was used as a mode TCM.After optimizing the setting parameters of SWATH,rolling collision energy(CE)and variable Q1 isolation windows were found to be more efficient for sanguisorbin identification than the fixed CE and fixed Q1 isolation window.More importantly,the qualitative efficiency of SWATH-MS on sanguisorbins was found significantly higher than that of IDA-MS data acquisition.In IDA mode,18 kinds of sanguisorbins were detected in sanguisorbin extract.A total of 47 sanguisorbins were detected when SWATH-MS was used under rolling CE and flexible Q1 isolation window modes.Besides,26 metabolites of sanguisorbins were identified in rat plasma,and their metabolic pathways could be deduced as decarbonylation,oxidization,reduction,methylation,and glucuronidation according to their fragmental ions acquired in SWATH-MS mode.Thus,SWATH-MS data acquisition could provide more comprehensive information for the component and metabolite identification for TCMs than IDA-MS.
基金supported by the National Key Research and Development Program of China(2023YFD1800100 to Feng X and Bai Y)the National Natural Science Foundation of China(22177031 to Feng X,92163127 to Bai Y,82102415 to Wan M,and 82304277 to Zhang C)+4 种基金the Natural Science Foundation of Hunan Province(2024JJ4007 and 2024RC3078 to Feng X,2022RC1107 and 2024JJ2010 to Bai Y)the Natural Science Foundation of Changsha(kq2208050 to Zhang C)the Health and Medical Research Fund(HMRF),Hong Kong SAR(22210412to Wong WL)the Independent Research Project of the College of Advanced Interdisciplinary Studies of NUDT(22-ZZKY-03 to Pu H)the Project of Hunan Provincial Key Laboratory of Anti-Resistance Microbial Drugs(2023TP1013)。
文摘The global antibiotic resistance crisis necessitates urgent solutions.One innovative approach involves potentiating antibiotics and non-antibiotic drugs with adjuvants or boosters.A major drawback of these membrane-active boosters is their limited biocompatibility,as they struggle to differentiate between prokaryotic and eukaryotic membranes.This study reports the chemical biology investigation of a dual-action oligoamidine(OA1)booster with a glutathione-triggered decomposition mechanism.OA1,when combined with other antimicrobial molecules,exhibits a triple-targeting mechanism including cell membrane disruption,DNA targeting,and intracellular enzyme inhibition.This multi-targeting mechanism not only enhances the in vitro and in vivo eradication of antibiotic-resistant“ESKAPE”pathogens,but also suppresses the development of bacterial resistance.Furthermore,OA1 maintains its activity in bacterial cells by creating an oxidative environment,while it quickly decomposes in mammalian cells due to high glutathione levels.These mechanistic insights and design principles may provide a feasible approach to develop novel antimicrobial agents and effective anti-resistance combination therapies.