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LADA strategy for the synthesis of unnatural amino acids and direct modifications of peptides

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Science China Chemistry 2023年第6期66卷 1788-1794页

作者： Jun-Liang Zhou yun-qi liu Zhan-Kui Sun Shanghai Frontiers Science Center for Drug Target Identification and Drug Delivery School of Pharmaceutical SciencesShanghai Jiao Tong UniversityShanghai 200240China Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Pharm-X CenterSchool of Pharmaceutical SciencesShanghai Jiao Tong UniversityShanghai 200240China AI Pharma Center Zhangjiang Institute for Advanced StudyShanghai Jiao Tong UniversityShanghai 200240China Shanghai Artificial Intelligence Laboratory Shanghai 200232China

Unnatural amino acids(UAAs)are important building blocks in organic synthesis and drug discovery.They are also frequently integrated into peptides or proteins for biological studies.However,the direct and simplified synthesis of UAAs remains a great challenge.At the same time,vast known peptide modifications are based on carbon-heteroatom bonds.There are no general methods for peptide modifications via the construction of C–C bonds.To address this challenge,herein we propose the LADA strategy,which is composed of two steps:the selective labeling and activation of cysteine residues,the desulfurization to generate carbon-centered radical and the radical addition to alkenes to build C–C bond.This one-pot protocol has obvious advantages such as good functional group tolerance,biocompatible reaction conditions,and retained stereochemistry.This strategy was successfully utilized for the synthesis of unnatural amino acids and direct modifications of peptides.

关键词： unnatural amino acids peptide modifications desulfurization cysteine radical addition

Diketopyrrolopyrrole-based Conjugated Polymers as Representative Semiconductors for High-Performance Organic Thin-Film Transistors and Circuits

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Chinese Journal of Polymer Science 2023年第5期41卷 671-682,I0006页

作者： Kai-qing liu Yuan-He Gu Zheng-Ran Yi yun-qi liu Zhuhai Fudan Innovation Institution Zhuhai 518057China Department of Environmental Science and Engineering Faculty of Innovation EngineeringMacao University of Science and TechnologyMacao 999078China Key Laboratory of Organic Solids Beijing National Laboratory for Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Since the first report of diketopyrrolopyrrole(DPP)-based conjugated polymers for organic thin-film transistors(OTFTs),these polymers have attracted great attention as representative semiconductors in high-performance OTFTs.Through unremitting efforts in molecular-structure regulation and device optimization,significant mobilities exceeding 10 cm2·V–1·s–1 have been achieved in OTFTs,greatly promoting the applied development of organic circuits.In this review,we summarize our progress in molecular design,synthesis and solution-processing of DPP-based conjugated polymers for OTFT devices and circuits,focusing on the roles of design strategies,synthesis methods and processing techniques.Furthermore,the remaining issues and future outlook in the field are briefly discussed.

关键词： Diketopyrrolopyrrole Polymer semiconductors Organic thin-film transistor Organic circuits

New insights into the mechanism of reactive adsorption desulfurization on Ni/ZnO catalysts:Theoretical evidence showing the existence of interfacial sulfur transfer pathway and the essential role of hydrogen

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Petroleum Science 2023年第5期20卷 3240-3250页

作者： Hou-Yu Zhu Nai-You Shi Dong-Yuan liu Rui Li Jing-Gang Yu qi-Tang Ma Tu-Ya Li Hao Ren Yuan Pan yun-qi liu Wen-Yue Guo School of Materials Science and Engineering China University of Petroleum(East China)Qingdao266580ShandongChina State Key Laboratory of Heavy Oil Processing College of Chemistry and Chemical EngineeringChina University of Petroleum(East China)Qingdao266580ShandongChina

As well known in the petroleum industry and academia,Ni/ZnO catalysts have excellent desulfurization performance.However,the sulfur transfer mechanism of reactive adsorption desulfurization(RADS)that occurs on Ni/ZnO catalysts remains controversial.Herein,a periodic Ni nanorod supported on ZnO slab was built to represent the Ni/ZnO system,and density functional theory calculations were performed to study the sulfur transfer process and the role of H_(2)within the process.The results elucidate that the direct solid-state diffusion of S from Ni to interfacial oxygen vacancies(Ov)is more favorable than the hydrogenation of S to SH/H_(2)S on Ni and the subsequent H_(2)S desorption,and accordingly,H_(2)O is produced on Ni rather than on ZnO.Ab initio thermodynamics analysis shows that the hydrogen atmosphere applied in preparing Ni/ZnO catalysts greatly promotes the O_(v)formation on ZnO surface,which accounts for the presence of interfacial O_(v)in freshly prepared catalysts.Under RADS condition,hydrogenation of interfacial O atoms to form O-H groups facilitates the reverse spillover of these lattice O atoms from ZnO to Ni,accompanied with the interfacial O_(v)generation.In contrast to the classic S transfer mechanism via H_(2)S,the present work clearly demonstrates that the interfacial S transfer is a feasible reaction pathway in the RADS mechanism.More importantly,the existence of interfacial O_(v)is an essential prerequisite for this interfacial S diffusion,and H_(2)plays a key role in facilitating the O_(v)formation.

关键词： Reactive adsorption desulfurization Ni/ZnO Interface Sulfur transfer Density functional theory

A FUNCTIONAL CONJUGATED HYPERBRANCHED POLYMER DERIVED FROM TETRAPHENYLETHENE AND OXADIAZOLE MOIETIES:SYNTHESIS BY ONE-POT “A_4+B_2+C_2” POLYMERIZATION AND APPLICAION AS EXPLOSIVE CHEMOSENSOR AND PLED

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Chinese Journal of Polymer Science 2013年第10期31卷 1432-1442页

作者： Wen-bo Wu Shang-hui Ye Li-jin Huang Gui Yu yun-qi liu Jin-gui qin Zhen Lia Department of Chemistry Hubei Key Lab on Organic and Polymeric Opto-Electronic MaterialsWuhan University Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences

A new conjugated hyperbranched polymer （hb-TFO） containing tetraphenylethylene （TPE） units, a famous aggregation-induced emission （AIE） active group, as the core, was synthesized successfully with modest yield via one-pot Suzuki polymerization reaction. Thanks to the introduction of TPE moieties, hb-TFO exhibited aggregation-enhanced emission （AEE） property, and could work as explosive chemosensor with high sensitivity. The polymeric light-emitting diode （PLED） device was fabricated to investigate its electroluminescent property, and hb-TFO demonstrated a maximum luminance efficiency of 0.22 cd/A and a maximum brightness of 545 cd/m2 at 15.9 V.

关键词： Hyperbranched polymer AEE TPE Explosive chemosensor PLED.

STUDY ON THE SYNTHESIS OF 1,3,4,6-TETRATHIAPENTALENE-2,5-DIONE(THIAPENDIONE)

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Chinese Chemical Letters 1995年第5期6卷 363-366页

作者： Sheng Gao liu Pei Ji WU yun qi liu and Dao Ben ZHU (Institute of Chemistry, Academia Sinica, Beijing 100080) Acad Sinica Inst Chem Beijing 100080 Peoples R China

Synthesis of 1,3,4,6-tetrathiapentalene-2,5-dione(thiapendione) has been studied in detail and a convenient synthetic procedure is reported.

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Synthesis of a Novel Copper Phthalocyanine-Fullerene Dyad

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Chinese Chemical Letters 1997年第9期8卷 811-814页

作者： Wen Feng qiUa yun qi liu Cai Yuan PAN Dao Ben ZHU(Institute of Chemistry, Chinese Academy of Sciences, Beijing 100080 Department of Material Science and Engineering, the University of Scienceand Technology of China, Hefei 230026) Institute of Chemistry Chinese Academy of Sciences Beijing 100080 China Department of Material Science Univ. of Sci./Technology of China Hefei 230026 China

A new copper phthalocyanine-fullerene dyad (CuPc-C-60) was synthesized by Diels-Alder adduct of corresponding CuPc and C-60. The chemical structure of this compound was characterized by elemental analysis, MS, IR, UV-... 详细信息

关键词： Synthesis of a Novel Copper Phthalocyanine-Fullerene Dyad

Progress of nanoscience in China

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Frontiers of physics 2014年第3期9卷 257-288页

作者： Yu-Liang Zhao Yan-Lin Song Wei-Guo Song Wei Liang Xing-Yu Jiang Zhi-Yong Tang Hong-Xing Xu Zhi-Xiang Wei yun-qi liu Ming-Hua liu Lei Jiang Xin-He Bao Li-Jun Wan Chun-Li Bai National Center for Nanoscience and Nanotechnology Beijing 100190 China Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Institute of Physics Chinese Academy of Sciences Beijing 100190 China Institute of High Energy Physics Chinese Academy of Sciences Beijing 100039 China Institute of Biophysics Chinese Academy of Sciences Beijing 100190 China School of Chemistry and Environment Beijing University of Aeronautics and Astronautics Beijing 100191 China Shenyang Branch Chinese Academy of Seienees Shenyang 110004 China Chinese Academy of Sciences Beijing 100864 China

Fast evolving nanoseienees and nanotechnology in China has made it one of the front countries of nanotechnology development. Ill this review, we summarize some most recent progresses in nanoseienee research and nanotechnology development in China. The topics we selected in this article include llano-fabrication, nanocatalysis, bioinspired nanoteehnology, green printing nanotechnology, nanoplasmonics, nanomedicine, nanomaterials and their applications, energy and environmental nanoteehnology, nano EHS （nanosafety）, etc. Most of them have great potentials in applications or application-related key issues in future.

关键词： nanoscience nanotechnology nanomaterials nanomedicine plasmonics fal）rication catalysis nano EHS （nanosafety）

Synergistic effect of hyperbaric oxygen preconditioning and hydrogen-rich saline in ameliorating rat flap ischemia/reperfusion injury

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Plastic and Aesthetic Research 2015年第1期2卷 332-339页

作者： Yi-Ding Xiao yun-qi liu Ming-Zi Zhang You-Bin Wang Yi-Fang liu Xue-Mei Ma Department of Plastic Surgery Peking Union Medical College HospitalDongcheng 100730BeijingChina College of Life Science and Bioengineering Beijing University of TechnologyChaoyang 100124BeijingChina

Aim:This study was conducted to evaluate the synergistic effects of hyperbaric oxygen(HBO)preconditioning and hydrogen-rich saline(HRS)treatment on skin flap survival and apoptosis in a rat ischemia/reperfusion(IR)skin flap model.Methods:Male Sprague-Dawley rats were randomly divided into five groups:one sham surgery group(sham group)and four surgery groups(IR group,HBO group,HRS group,and HBO+HRS group).An extended epigastric adipocutaneous flap(6 cm×9 cm)was raised over the abdomen in each animal of all five groups.The last four groups underwent 6 h of IR management and were treated,respectively,with normal saline,HBO,HRS(HRS,0.8 mmol/L),or a combined approach(HBO and HRS).On the 3rd postoperative day,flap survival rate and perfusion condition,apoptotic index,caspase-3 activity,protein expression of pASK1 and Bcl-2/Bax ratio,and Bcl-2 messenger RNA(mRNA)expression were assessed.Results:Prior studies have shown the protective effects of HBO and HRS,both of which have been associated with an increase in flap survival.Compared to the IR group,the flaps in the HBO,HRS,and HBO+HRS groups showed better perfusion and a larger survival area with a low number of apoptotic cells,low caspase-3 activity and pASK1 expression,and a high Bcl-2/Bax ratio and Bcl-2 mRNA expression.Of these groups,the HBO+HRS group showed the best flap survival.Conclusion:Both HBO and HRS treatments increase the rate of flap survival,while the synergistic application of HBO and HRS showed a higher survival rate as compared to individual treatments of each.The potential regulation of apoptosis with the use of these two modalities may improve skin flap survival.

关键词： Apoptosis hydrogen‑rich saline hyperbaric oxygen ischemia/reperfusion injury skin flaps

A functionalized activated carbon adsorbent prepared from waste amidoxime resin by modifying with H_(3)PO_(4) and ZnCl_(2) and its excellent Cr(Ⅵ)adsorption

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International Journal of Minerals,Metallurgy and Materials 2024年第3期31卷 585-598页

作者： Chunlin He yun liu Mingwei qi Zunzhang liu Yuezhou Wei Toyohisa Fujita Guifang Wang Shaojian Ma Wenchao Yang School of Resources Environment and MaterialsGuangxi UniversityNanning 530004China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi UniversityNanning 530004China School of Nuclear Science and Technology University of South ChinaHengyang 421000China School of Nuclear Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China Key Laboratory of New Low-carbon Green Chemical Technology Education Department of Guangxi Zhuang Autonomous RegionNanning 530004China

With the application of resins in various fields, numerous waste resins that are difficult to treat have been produced. The industrial wastewater containing Cr(Ⅵ) has severely polluted soil and groundwater environments, thereby endangering human health. Therefore, in this paper, a novel functionalized mesoporous adsorbent PPR-Z was synthesized from waste amidoxime resin for adsorbing Cr(Ⅵ). The waste amidoxime resin was first modified with H3PO4 and ZnCl_(2), and subsequently, it was carbonized through slow thermal decomposition. The static adsorption of PPR-Z conforms to the pseudo-second-order kinetic model and Langmuir isotherm, indicating that the Cr(Ⅵ) adsorption by PPR-Z is mostly chemical adsorption and exhibits single-layer adsorption. The saturated adsorption capacity of the adsorbent for Cr(Ⅵ) could reach 255.86 mg/g. The adsorbent could effectively reduce Cr(Ⅵ) to Cr(Ⅲ) and decrease the toxicity of Cr(Ⅵ) during adsorption. PPR-Z exhibited Cr(Ⅵ) selectivity in electroplating wastewater. The main mechanisms involved in the Cr(Ⅵ) adsorption are the chemical reduction of Cr(Ⅵ) into Cr(Ⅲ) and electrostatic and coordination interactions. Preparation of PPR-Z not only solves the problem of waste resin treatment but also effectively controls Cr(Ⅵ) pollution and realizes the concept of “treating waste with waste”.

关键词： waste amidoxime resin mesoporous adsorbent H_(3)PO_(4)and ZnCl_(2)processing Cr(VI)adsorption electroplating wastewater