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Rapid Determination of Endogenous 20-Hydroxyecdysone in Plants on MALDI-TOF/TOF Mass Spectrometry via Chemical Labeling Based on Boronate Affinity

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Journal of Analysis and Testing 2022年第3期6卷 318-326页

作者： Ya-Shun Chen yu-qi feng College of Science Honghe UniversityMengzi 661100China Department of Chemistry Wuhan UniversityWuhan 430072China

20-Hydroxyecdysone(20E)derived from plants has a wide range of physiological and pharmacological ef ects on animals and humans,and rapid and sensitive methods for screening of the endogenous 20E in plants are thus ***,a matrixassisted laser desorption/ionization time-of-f ight tandem mass spectrometry(MALDI-TOF/TOF MS)method is described for rapid and sensitive determination of endogenous 20E in *** is based on the use of the(3-(acridin-9-ylamino)phenyl)boronic acid(AYPBA)as the mass tag to assist the MS and tandem MS(MS^(n))analysis of 20E on MALDI-TOF/TOF *** linearity was obtained with a determination coef cient(R^(2))larger than 0.99 in the range of 0.025–2.5μΜ.The limit of detection(LOD)was 2.4 *** precision and accuracy were gained by intra-and inter-day analysis with relative standard deviations less than 19.5%and relative recoveries ranging from 85.7 to 105.2%.In addition,the AYPBA labeled 20E produced abundant characteristic fragment ions under the high energy collision-induced dissociation,which facilitated the identif cation of 20E by MS^(2)analysis on MALDI-TOF/TOF *** the method,we enabled the identif cation and quantif cation of endogenous 20E in four herbs including Cyanotis arachoidea,Achyranthes bidentata,Spinacia oleracea and Chenopodium quinoa willd.,demonstrating the feasibility of the proposed method for screening of the endogenous 20E in plants.

关键词： Matrix-assisted laser desorption/ionization time-of-flight tandem mass spectrometry 20-Hydroxyecdysone Chemical labeling Boronate affinity

Sandwich structure for enhancing the interface reaction of hexanitrohexaazaisowurtzitane and nanoporous carbon scaffolds film to improve the thermal decomposition performance

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Defence Technology（防务技术） 2022年第10期18卷 1886-1894页

作者： Shuai-da Zhu Zi-chen Hu yu-qi Cao Xiao-xia Li yu-qi feng Xiong Cao Peng Deng Shanxi Fire&Explosion-Proofing Safety Engineering and Technology Research Center North University of ChinaTaiyuan030051PR China State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing100081PR China

Improving the thermal decomposition performance of hexanitrohexaazaisowurtzitane(CL-20)by appropriate methods is helpful to promote the combustion performance of CL-20-based solid *** this study,we synthesized a sandwich structure of CL-20 and nanoporous carbon scaffolds film(NCS)and emphatically studied the thermal decomposition performance of the composite *** analysis and differential scanning calorimetry were used to measure the thermal decomposition process of the composite *** kinetic parameters of thermal decomposition were calculated by the thermal dynamic analysis software *** results showed that the thermal decomposition performance of the sandwich structure of CL-20 and NCS was better than *** the tested samples,NCS with a pore size of 15 nm had the best catalytic activity for the thermal decomposition of ***,the thermal decomposition curve of the composite structure at the heating rate of 1 K/min was deconvoluted by mathematical method to study the thermal decomposition *** a possible catalytic mechanism was *** excellent thermal decomposition performance is due to the sandwich structure enhances the interface reaction of CL-20 and *** work may promote the extensive use of CL-20 in the field of solid rocket propellant.

关键词： CL-20 NCS Catalysis Thermal decomposition Sandwich structure

Site-specific quantification of 5-carboxylcytosine in DNA by chemical conversion coupled with ligation-based PCR

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Chinese Chemical Letters 2021年第11期32卷 3426-3430页

作者： qian Wang Jiang-Hui Ding Jun Xiong Yang feng Bi-feng yuan yu-qi feng Sauvage Center for Molecular Sciences Department of ChemistryWuhan UniversityWuhan 430072China School of Health Sciences Wuhan UniversityWuhan 430071China

5-Methylcytosine(5mC)is the most important epigenetic modification in *** active DNA demethylation could be achieved through the ten-eleven translocation(TET)protein-mediated oxidization of 5mC with the generation of 5-hydroxymethylcytosine(5hmC),5-formylcytosine(5fC)and 5-carboxylcytosine(5caC).It has been known that 5mC,5hmC and 5fC play critical roles in modulating gene ***,unlike the 5mC,5hmC,and 5fC,the functions of 5caC are still *** of the functions of 5caC relies on the accurate quantification and localization analysis of 5caC in *** the current study,we developed a method by chemical conversion in conjugation with ligation-based real-time quantitative PCR(qPCR)for the site-specific quantification of 5caC in *** method depends on the selective conversion of 5caC to form dihydrouracil(DHU)by pyridine borane *** behaves like thymine and pairs with adenine(DHU-A).Thus,the chemical conversion by pyridine borane leads to the transformation of base paring from 5caC-G to DHU-A,which is utilized to achieve the site-specific detection and quantification of 5caC in *** a proof-of-concept,the developed method was successfully applied in the site-specific quantification of 5caC in synthesized DNA spiked in complex biological *** method is rapid,straightforward and cost-effective,and shows promising in promoting the investigation of the functional roles of 5caC in future study.

关键词： 5-Methylcytosine 5-Carboxylcytidine Dihydrouracil Mass spectrometry PCR Chemical conversion

Simultaneous determination of indole metabolites of tryptophan in rat feces by chemical labeling assisted liquid chromatography-tandem mass spectrometry

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Chinese Chemical Letters 2022年第11期33卷 4746-4749页

作者： qin-feng Zhang Hua-Ming Xiao Jin-Tao Zhan Bi-feng yuan yu-qi feng Department of Chemistry Wuhan UniversityWuhan 430072China School of Public Health Wuhan UniversityWuhan 430071China

As the connecting part of diet and host physiology,intestinal microbes can convert the ingested diet into a huge number of physiologically active small *** metabolites of tryptophan are precursors or signal molecules for many biologically active substances,which are involved in serotonin and microbial catabolism *** understand the influence of tryptophan metabolism in the intestinal environment on the neurological and immune systems at the molecular level,it is important to establish a high-coverage analytical method to comprehensively analyze the metabolites involved in tryptophan ***,due to a small molecular weight and poor response during mass spectrometry analysis,as well as weak retention on the reversed-phase chromatography,determination of indole metabolites of tryptophan is ***,we proposed a method for the simultaneous determination of 20 indole metabolites of tryptophan in a single run on reversed-phase chromatography by chemical labeling coupled to liquid chromatography-tandem mass spectrometry analysis.4-(Dimethylamino)benzaldehyde(DMAB)was used for the labeling of indole metabolites of tryptophan,which could significantly improve the detection sensitivities and retention of these metabolites on reversed-phase *** the developed method,we realized the sensitive detection and comprehensive analysis of 15 endogenous indole metabolites of tryptophan in rat feces samples with functional dyspepsia intervention by *** developed method offers a useful tool for studying tryptophan metabolism-related diseases.

关键词： Chemical labeling Liquid chromatography-mass spectrometry Indole metabolites Tryptophan Rat feces

Comprehensive profiling and evaluation of the alteration of RNA modifications in thyroid carcinoma by liquid chromatography-tandem mass spectrometry

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Chinese Chemical Letters 2022年第8期33卷 3772-3776页

作者： Meng-yuan Chen Chu-Bo qi Xiao-Meng Tang Jiang-Hui Ding Bi-feng yuan yu-qi feng School of Public Health Wuhan UniversityWuhan 430071China Department of Chemistry Sauvage Center for Molecular SciencesWuhan UniversityWuhan 430072China Jiangxi Provincial People's Hospital Affiliated to Nanchang University Nanchang 330006China

RNA molecules contain diverse modifications that display important functions in a variety of physiological and pathological *** far over 150 chemical modifications have been characterized to be present in various RNA species,such as in messenger RNA(mRNA),ribosomal RNA(rRNA),and transfer RNA(tRNA).Previous studies revealed that certain RNA modifications were correlated to specific human diseases,indicating RNA modifications could serve as the potential indicator of human ***,systemic investigation of the alteration of RNA modifications in different RNA species of carcinoma tissues are still ***,we carried out the comprehensive profiling and evaluation of the alteration of RNA modifications in thyroid carcinoma by liquid chromatography-tandem mass spectrometry(LC-ESIMS/MS)*** developed method allowed us to simultaneously detect 48 different types of RNA *** this method,we detected 10,15,14,and 25 modifications in m RNA,18 S r RNA,28 S rRNA and small RNA(<200 nt),*** to the normal tissues,we revealed a total of 14 RNA modification exhibited significant increase and 2 RNA modifications showed significant decrease in thyroid carcinoma *** study provided the first comprehensive profile as well as the alteration of modifications in different RNA species in thyroid carcinoma and matched tumor-adjacent normal *** altered pattern RNA modifications may serve as the indicator of thyroid ***,this study may promote the in-depth understanding of the regulatory roles of RNA modifications in thyroid carcinoma.

关键词： RNA modification Liquid chromatography-mass spectrometry Thyroid carcinoma Profiling

Chiral derivatization coupled with liquid chromatography/mass spectrometry for determining ketone metabolites of hydroxybutyrate enantiomers

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Chinese Chemical Letters 2018年第1期29卷 115-118页

作者： qing-yun Cheng Jun Xiong Fang Wang Bi-feng yuan yu-qi feng Key Laboratory of Analytical Chemistry for Biology and Medicine (Ministry of Education) Department of Chemistry Wuhan University Department of Pharmacy Dingxi Campus Gansu University of Traditional Chinese Medicine

Ketone bodies are small lipid-derived molecules and the metabolism of ketone bodies interfaces with various physiological processes. 3-Hydroxybutyric acid （3HB） is the most stable ketone body and can be employed to supply energy source. 2-Hydroxybutyric acid （2HB）, an isomer of 3HB, was demonstrated to be an early biomarker for both insulin resistance and impaired glucose regulation. Both 2HB and 3HB are chiral carboxylic acids and exist in two steric configurations （D/L-2HB and D/L-3HB）. It is difficult for these enantiomers to be differentiated by routine analytical methods In the current study, we developed a strategy by chiral derivatization coupled with liquid chromatography/mass spectrometry （LC-ESI-MS） analysis for simultaneous determination of D-2HB, L-2HB, D-3HB and L-3HB enantiomers. （5）-（＋）-l-（2- Pyrrolidinylmethyl）-pyrrolidine （PMP） was used for efficient labeling of HBs. Our results showed that the retention behavior of D/L-2HB and D/L-3HB enantiomers was greatly improved after labeling by PMP and the four derivatives can be distinctly separated on C18 reversed-phase column. Moreover, PMP chiral derivatization greatly enhanced the detection sensitivities of HBs up to 55.3 folds because of the introduction of easily ionizable tertiary amino group. Using this method, we simultaneously quantified D-2HB, L-2HB, D-3HB, and L-3HB enantiomers in human renal cell carcinoma （RCC） tissues and the tumor adjacent normal tissues. The result demonstrated that both D-3HB and L-3HB can be detected in human renal tissues, however, only L-2HB was detected in human renal tissues. In addition, the quantification results showed that the contents of D-3HB were approximate 10 folds higher than L-3HB. Taken together, the developed method offered an efficient approach for the sensitive analysis of D/L-2HB and D/L-3HB enantiomers, which may facilitate the in-depth study of the functions of HBs.

关键词： 2-Hydroxybutyric acid3-Hydroxybutyric acidEnantiomerChiral derivatizationMass spectrometry

Sensitive determination of inosine RNA modification in single cell by chemical derivatization coupled with mass spectrometry analysis

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Chinese Chemical Letters 2023年第10期34卷 98-101页

作者： Wan-Bing Tao Neng-Bin Xie qing-yun Cheng yu-qi feng Bi-feng yuan College of Chemistry and Molecular Sciences Department of Radiation and Medical OncologyZhongnan Hospital of Wuhan UniversityWuhan UniversityWuhan 430071China School of Public Health Wuhan UniversityWuhan 430071China Research Center of Public Health Renmin Hospital of Wuhan UniversityWuhan 430060China Cancer Precision Diagnosis and Treatment and Translational Medicine Hubei Engineering Research Center Zhongnan Hospital of Wuhan UniversityWuhan Research Center for Infectious Diseases and CancerChinese Academy of Medical SciencesWuhan 430071China

Inosine is a vital RNA modification across three kingdoms of *** has been demonstrated that inosine plays important roles in modulation of the fate of *** the current study,we developed a highly sensitive method to determine inosine in a single cell by N-cyclohexyl-N’-β-(4-methylmorpholinium)ethylcarbodiimide p-toluenesulfonate(CMCT)derivatization in combination with mass spectrometry *** results showed that the detection sensitivity of inosine was increased by 556-fold after CMCT derivatization,with the limit of detection(LOD)being 4.5 *** the established method,we could detect inosine from 13.0 pg of total RNA of HEK293T ***,inosine in RNA from a single cell could also be clearly detected due to the improved detection ***,we found the level of inosine in RNA of sleep-deprived mice was significantly increased compared to the control mice,indicating that inosine is associated with sleep behavior and might be a potential indicator of sleep *** together,the chemical derivatization coupled with mass spectrometry analysis offers a valuable tool in determination of endogenous RNA modifications in a single cell,which should benefit the functional study of RNA modification in rare clinical samples.

关键词： Inosine RNA modification CMCT Derivatization Mass spectrometry Single cell

Chronic sleep deprivation induces alterations in DNA and RNA modifications by liquid chromatography-mass spectrometry analysis

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Chinese Chemical Letters 2024年第8期35卷 413-417页

作者： Tian feng yun-Ling Gao Di Hu Ke-yu yuan Shu-Yi Gu Yao-Hua Gu Si-yu yu Jun Xiong yu-qi feng Jie Wang Bi-feng yuan School of Public Health Research Center of Public HealthRenmin Hospital of Wuhan UniversityWuhan UniversityWuhan 430071China Department of Radiation and Medical Oncology Zhongnan Hospital of Wuhan UniversityWuhan UniversityWuhan 430071China Key Laboratory of Magnetic Resonance in Biological Systems State Key Laboratory of Magnetic Resonance and Atomic and Molecular PhysicsNational Center for Magnetic Resonance in WuhanWuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of Sciences-Wuhan National Laboratory for OptoelectronicsWuhan 430071China University of Chinese Academy of Sciences Beijing 101408China Institute of Neuroscience and Brain Diseases Xiangyang Central HospitalAffiliated Hospital of Hubei University of Arts and ScienceXiangyang 441000China Phase I Clinical Trial Laboratory Zhongnan Hospital of Wuhan UniversityWuhan 430071China

Sleep deprivation(SD)is a widespread issue that disrupts the lives of millions of *** effects ini-tiate as changes within neurons,specifically at the DNA and RNA level,leading to disruptions in neuronal plasticity and the dysregulation of various cognitive functions,such as learning and *** acid epigenetic modifications that could regulate gene expression have been reported to play crucial roles in this ***,there is a lack of comprehensive research on the correlation of SD with nucleic acid epigenetic *** the current study,we aimed to systematically investigate the landscape of modifications in DNA as well as in small RNA molecules across multiple tissues,including the heart,liver,kidney,lung,hippocampus,and spleen,in response to chronic sleep deprivation(CSD).Using liquid chromatography-tandem mass spectrometry(LC-MS/MS)analysis,we characterized the dynamic changes in DNA and RNA modification profiles in different tissues of mice under CSD ***,we ob-served a significant decrease in the level of 5-methylcytosine(5mC)and a significant increase in the level of 5-hydroxymethylcytosine(5hmC)in the kidney in CSD *** RNA modifications,we observed an overall increased trend for most of these significantly changed modifications across six tis-sues in CSD *** study sheds light on the significance of DNA and RNA modifications as crucial epigenetic markers in the context of CSD-induced stress.

关键词： Sleep deprivation Epigenetics Mass spectrometry DNA modification RNA modification Small RNA

6-Thioguanine incorporates into RNA and induces adenosine-to-inosine editing in acute lymphoblastic leukemia cells

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Chinese Chemical Letters 2023年第1期34卷 539-543页

作者： Xue-Jiao You Lin Li Tong-Tong Ji Neng-Bin Xie Bi-feng yuan yu-qi feng Department of Chemistry Sauvage Center for Molecular SciencesWuhan UniversityWuhan 430072China School of Public Health Wuhan UniversityWuhan 430071China School of Pharmacy Shanghai Jiao Tong UniversityShanghai 200240China

6-Thioguanine(6TG)is a widely used chemotherapeutic agent for the treatment of a variety of human diseases including acute lymphoblastic *** entry into cells,6TG is metabolically converted into 6-thioguanosine(^(S)G)nucleotide that can be incorporated into the genome during DNA replication.^(S)G in genomic DNA could induce cell death by triggering the post-replicative mismatch repair(MMR)***,incorporation of 6TG into the Cp G sites could perturb the global DNA methylation and gene ***,the effect of 6TG on RNA modifications is still ***-toinosine(A-to-I)editing in RNA is one of the most common post-transcriptional modifications in mammals and there is growing evidence showing the significant alteration of A-to-I RNA editing in tumor tissues compared to normal *** the current study,we examined the incorporation of 6TG into RNA and investigated its effect on A-to-I editing of bladder cancer-associated protein(BLCAP)transcript in acute lymphoblastic leukemia *** results demonstrated that ^(S)G could be incorporated into various RNA species,with m RNA having the most abundant ^(S)*** addition,the results showed 6TG treatment elevated A-to-I editing in BLCAP transcript through upregulating adenosine deaminase 2 acting on RNA(ADAR2),which eventually contributes to the decreased cell *** study highlights a new mechanism of the cytotoxicity of 6TG in inducing cell death.

关键词： 6-Thioguanine RNA modification Inosine Leukemia Mass spectrometry