亮氨酸-脑啡肽结合H<sup>+</sup>和Li<sup>+</sup>的氢氘交换实验与理论研究

引用本文: 陈银娟, 熊行创, 李振华, 江游, 方向, 戴新华, 丁传凡. 亮氨酸-脑啡肽结合H⁺和Li⁺的氢氘交换实验与理论研究[J]. 分析化学, 2018, 46(4): 556-562. doi: 10.11895/j.issn.0253-3820.171479 shu

Citation: CHEN Yin-Juan, XIONG Xing-Chuang, LI Zhen-Hua, JIANG You, FANG Xiang, DAI Xin-Hua, DING Chuan-Fan. Investigation of Protonated and Lithiated Leucine-Enkephalin by Hydrogen/Deuterium Exchange and Theoretical Calculations[J]. Chinese Journal of Analytical Chemistry, 2018, 46(4): 556-562. doi: 10.11895/j.issn.0253-3820.171479 shu

亮氨酸-脑啡肽结合H⁺和Li⁺的氢氘交换实验与理论研究

陈银娟 ^1,2, ,
熊行创 ^3, ,
李振华 ^2, ,
江游 ^3, ,
方向 ^3, ,
戴新华 ^3, ,
丁传凡 ^2,

1.
同济大学化学科学与工程学院, 上海 200092;
2.
复旦大学化学系, 上海 200433;
3.
中国计量科学研究院化学计量与分析科学研究所, 北京 100013
基金项目:
本文系国家自然科学基金项目（Nos.21773035，21605135）和国家重大仪器设备开发专项（No.2012YQ22011307）资助

摘要: 气相氢氘交换质谱（HDX-MS）实验与量子化学计算结合，比较了亮氨酸-脑啡肽（YGGFL）结合H⁺和Li⁺的反应和结构差异性。HDX-MS结果表明，在相同的实验条件下，[YGGFL+Li]⁺在交换5个氢原子后，氢氘同位素反应趋于停止，而[YGGFL+H]⁺上的9个可交换氢原子均可发生交换。这表明Li⁺会降低脑啡肽的氢氘交换率。理论计算发现，两种离子具有不同的最稳定结构：Li⁺与脑啡肽肽上的4个羰基氧原子结合能量最低，而脑啡肽氨基端发生质子化后产生最稳定的[YGGFL+H]⁺。基于此稳定结构，实验进一步从离子结构差异性和质子亲和势等方面对HDX实验结果进行了分析。

关键词:

English

Investigation of Protonated and Lithiated Leucine-Enkephalin by Hydrogen/Deuterium Exchange and Theoretical Calculations

1.
School of Chemical Science and Engineering, Tongji University, Shanghai 200092, China;
2.
Department of Chemistry, Fudan University, Shanghai 200433, China;
3.
Chemical Metrology & Analytical Science Division, National Institute of Metrology, Beijing 100013, China
Received Date: 05 December 2017
Revised Date: 09 January 2018
Fund Project:
This work was supported by the National Natural Science Foundation of China (Nos.21773035, 21605135) and the Ministry of Science and Techndogy of China (No.2012YQ22011307).

Abstract: Differences of protonated and lithiated leucine-enkephalin(LE) were investigated by hydrogen deuterium exchange-mass spectrometry (HDX-MS) combined with quantum chemistry calculation. The results revealed that the protonated ions possessed very high product yield with all hydrogen atoms being exchanged, while the reaction of lithiated LE stopped after exchanging five hydrogen atoms in the same experimental conditions. The different HDX behaviours probably indicated their conformational differences. To further clarify the experimental results, the most stable conformations of protonated and lithiated leucine-enkephalin were calculated by density functional theory. It was found that terminal amino group was the most thermodynamically stable protonation site, while Li⁺ in coordination of four carbonyl oxygen atoms formed the most favourable lithiated LE. The reaction field reduction of lithium LE was probably due to the less acidity of hydrogen atoms and the increasing rigid conformation change induced by lithium ion.

Key words:

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亮氨酸-脑啡肽结合H⁺和Li⁺的氢氘交换实验与理论研究

English

Investigation of Protonated and Lithiated Leucine-Enkephalin by Hydrogen/Deuterium Exchange and Theoretical Calculations

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

亮氨酸-脑啡肽结合H+和Li+的氢氘交换实验与理论研究

English

Investigation of Protonated and Lithiated Leucine-Enkephalin by Hydrogen/Deuterium Exchange and Theoretical Calculations

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs