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Regioselective C-C bond cleavage/aminocarbonylation cascade under copper catalysis

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Science China Chemistry 2024年第11期67卷 3798-3806页

作者： qi-chao Shan Yan Zhao Yong Wu Hong-Fei Liu Xin-Hua Duan Li-Na Guo Department of Chemistry School of Chemistry Energy Research Center of Energy Storage Materials and Devices Ministry of EducationXi'an Jiaotong University State Key Laboratory of Applied Organic Chemistry Lanzhou University

A regioselective C-C bond cleavage/aminocarbonylation cascade is presented. In recent years, tremendous progress has been made in the alkoxyl radical-mediated C-C bond cleavage of unstrained monocarbocycles. In contrast, the deconstruction and functionalization of bicyclic skeletons has been less developed and has mainly focused on the ring expansion process. Inspired by the aromatization-driven C-C bond cleavage, here we demonstrate a ring-opening/aminocarbonylation cascade under copper catalysis, in which the formation of a stable γ-lactam or succinimide skeleton reverses the selectivity of C-C cleavage. Remarkably, the photo and thermal assistance is not required when the succinimide skeleton is formed during the ring opening process. DFT calculations revealed that this unexpected ring-opening process is thermodynamically and kinetically favourable.

关键词： C-C bond cleavage controllable regioselectivity aminocarbonylation bicyclic alkoxy radical

Nickel-catalyzed carbonylative four-component 1,4-dicarbofunctionalization of 1,3-enynes

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Science China Chemistry 2024年第6期67卷 2029-2038页

作者： Yan Zhao qi-chao Shan Hong Xin Pin Gao Xu Yang Xin-Hua Duan Li-Na Guo Department of Chemistry School of ChemistryXi’an Key Laboratory of Sustainable Energy Material Chemistry and Engineering Research Center of Energy StorageMaterials and DevicesMinistry of EducationXi’an Jiaotong UniversityXi’an710049China School of Electrical Engineering Xi’an Jiaotong UniversityXi’an710049China

An efficient Ni-catalyzed four-component 1,4-carbocarbonylation of 1,3-enynes with activated alkyl halides and arylboronic acids under atmospheric pressure of CO is *** tuning the electronic and steric effects of alkyl radicals,both electronrich and electron-deficient 1,3-enynes were compatible with this *** protocol features mild conditions,broad substrate scope,excellent functional group compatibility and facile gram-scale synthesis,providing a practical approach to the quaternary carbon center-containing allenyl *** study revealed that the acyl-NiIIspecies plays an important role in both the coupling and the alkyl radical generation processes.

关键词： Ni catalysis four-component 1 4-carbocarbonylation 1 3-enynes

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Photo-Responsive Carbon Capture over Metalloporphyrin-C_(60) Metal-Organic Frameworks via Charge-Transfer

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Research 2024年第3期2023卷 233-241页

作者： Shi-chao qi Zhen Sun Zhi-Hui Yang Yun-Jie Zhao Jia-Xin Li Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China.

Great efforts have been devoted to the study of photo-responsive adsorption,but its current methodology largely depends on the well-defined photochromic units and their photo-driven molecular ***,a methodology to fabricate nondeforming photo-responsive sorbents is successfully *** C_(60)-fullerene doping in metalloporphyrin metal-organic frameworks(PCN-M,M=Fe,Co,or Ni)and intensively interacting with the metalloporphyrin sites,effective charge-transfer can be achieved over the metalloporphyrin-C_(60) architectures once excited by the light at 350 to 780 *** electron density distribution and the resultant adsorption activity are thus changed by excited states,which are also stable enough to meet the timescale of microscopic adsorption *** charge-transfer over Co(II)-porphyrin-C_(60) is proved to be more efficient than the Fe(II)-and Ni(II)-porphyrin-C_(60) sites,as well as than all the metalloporphyrin sites,so the CO_(2) adsorption capacity(CAC;at 0°C and 1 bar)over the C_(60)-doped PCN-Co can be largely improved from 2.05 mmol g^(−1) in the darkness to 2.69 mmol g−1 with light,increased by 31%,in contrast to photo-irresponsive CAC over all C_(60)-undoped PCN-M sorbents and only the photo-loss CAC over C_(60).

关键词： porphyrin adsorption excited

Homochirality in Ferroelectrochemistry

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Chinese Journal of Chemistry 2024年第10期42卷 1133-1144页

作者： Hang Peng Jun-chao qi Yu-Si Liu Jia-Mei Zhang Wei-qiang Liao Ren-Gen Xiong Ordered Matter Science Research Center Nanchang UniversityNanchangJiangxi 330031China

What is the most favorite and original chemistry developed in your research group?We originally proposed the design principle for molecular ferroelectrics:ferroelectrochemistry,including quasi-spherical theory,the introduction of homochirality,and H/F *** changed the blind search for molecular ferroelectrics into targeted chemical design,which will develop into a new discipline.

关键词： Molecular ferroelectrics Homochirality Ferroelectricity Chemical design Point groups

Atomically dispersed calcium as solid strong base catalyst with high activity and stability

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Green Energy & Environment 2024年第10期9卷 1619-1626页

作者： Xiang-Bin Shao Zhi-Wei Xing Si-Yu Liu Ke-Xin Miao Shi-chao qi Song-Song Peng Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM)College of Chemical EngineeringNanjing Tech University30 South Puzhu Road

Solid strong base catalysts are highly attractive for diverse reactions owing to their advantages of neglectable corrosion,facile separation,and environmental ***,their widespread applications are impeded by basic components aggregation and low *** this work,we fabricate single calcium atoms on graphene （denoted as Ca1/G） by use of a redox strategy for the first time,producing solid strong base catalyst with high activity and *** precursor Ca（NO3）2is first reduced to CaO at 400℃ by the support graphene,forming CaO/G with conventional basic sites,and the subsequent reduction at 850℃ results in the generation of Ca1/G with atomically dispersed *** characterizations reveal that Ca single atoms are anchored on graphene in tetra-coordination （Ca–C2–N2） where N is in situ doped from Ca（NO3）*** atomically dispersed Ca,along with their anchoring on the support,endow Ca1/G with high activity and stability toward the transesterification reaction of ethylene carbonate with *** turnover frequency value reaches 128.0 h-1on Ca1/G,which is much higher than the traditional counterpart CaO/G and various reported solid strong bases (2.9–46.2 h-1).Moreover,the activity of Ca1/G is well maintained during 5 cycles,while 60% of activity is lost for the conventional analogue CaO/G due to the leaching of Ca.

关键词： Solid strong base Single Ca atoms Heterogeneous catalysts Transesterification Reaction

Efficacy and safety of Yiqi Peiyuan granules for improving the short-term prognosis of patients with acute kidney injury:A multicenter,double-blind,placebo-controlled,randomized trial

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Journal of Integrative Medicine 2024年第3期22卷 279-285页

作者： Jia-jia Wu Tian-yi Zhang Ying-hui qi Min-yan Zhu Yan Fang chao-jun qi Li-ou Cao Ji-fang Lu Bo-han Lu Lu-min Tang Jian-xiao Shen Shan Mou Department of Nephrology Molecular Cell Lab for Kidney DiseaseShanghai Peritoneal Dialysis Research CenterUremia Diagnosis and Treatment CenterRenji Hospital Affiliated to Shanghai Jiaotong University School of MedicineShanghai 200127China Department of Nephrology Shanghai Pudong New Area Punan HospitalShanghai 200125China Department of Nephrology Ningbo Hangzhou Bay HospitalNingbo 315336Zhejiang ProvinceChina

Background:Yiqi Peiyuan(YQPY)prescription,a composite prescription of traditional Chinese medicine,has been used to prevent or delay the continued deterioration of renal function after acute kidney injury(AKI)in some institutions and has shown considerable ***:This is the first randomized controlled trial to assess efficacy and safety of YQPY for improving short-term prognosis in adult patients with ***,setting,participants and interventions:This is a prospective,double-blind,multicenter,randomized,and placebo-controlled clinical trial.A total of 144 enrolled participants were randomly allocated to two groups according to a randomization ***,caregivers and investigators assessing the outcomes were blinded to group *** in the YQPY group received 36 g YQPY granules twice a day for 28 *** in the placebo group received a placebo in the same dose as the YQPY *** outcome measures:The primary outcome was the change in the estimated glomerular filtration rate(eGFR)between baseline and after 4 and 24 weeks of *** secondary outcomes were the change of serum creatinine(Scr)level between baseline and after treatment,and the incidence of endpoint events,defined as eGFR increasing by more than 25%above baseline,eGFR>75 mL/min per1.73 m2or the composite endpoint,which was defined as the sum of patients meeting either of the above ***:Data from a total of 114 patients(59 in the YQPY group and 55 in the control group)were *** mean changes in eGFR and Scr in weeks 4 and 24 had no difference between the two *** further subgroup analysis(22 in the YQPY group and 31 in the control group),the mean change in eGFR after treatment for 4 weeks was 27.39 mL/min per 1.73 m2in the YQPY group and 5.78 mL/min per1.73 m2in the placebo group,and the mean difference between groups was 21.61 mL/min per 1.73 m2(P<0.001).Thirteen(59.1%)patients in the YQPY group and 5(16.1%)in the placebo g

关键词： Chinese herbal medicine Randomized controlled trial Acute kidney injury Renal function

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Graphene-anchored sodium single atoms:A highly active and stable catalyst for transesterification reaction

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Nano Research 2024年第6期17卷 4979-4985页

作者： Song-Song Peng Yao Nian Xing-Ru Song Xiang-Bin Shao Chen Gu Zhi-Wei Xing Shi-chao qi Peng Tan You Han Xiao-qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech University30 South Puzhu RoadNanjing 211816China School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

Solid strong base catalysts have received considerable attention in various organic reactions due to their facile separation,neglectable corrosion,and environmental *** great progress has been made in the preparation of solid strong base catalysts,it is still challenging to avoid basic sites aggregation on support and active sites loss in reaction ***,we report a tandem redox strategy to prepare Na single atoms on graphene,producing a new kind of solid strong base catalyst(Na1/G).The base precursor NaNO_(3)was first reduced to Na2O by graphene(400℃)and successively to single atoms Na anchored on the graphene vacancies(800℃).Owing to the atomically dispersed of basicity,the resultant catalyst presents high activity toward the transesterification of methanol and ethylene carbonate to synthesize dimethyl carbonate(turnover frequency(TOF)value:125.7 h^(−1)),which is much better than the conventional counterpart Na2O/G and various reported solid strong bases(TOF:1.0-90.1 h^(−1)).Furthermore,thanks to the basicity anchored on graphene,the Na1/G catalyst shows excellent durability during *** work may provide a new direction for the development of solid strong base catalysts.

关键词： solid strong base catalyst basic sites redox graphene single Na atoms

典型重工业城市PM_(2.5)化学组成特征及来源解析

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中国环境科学 2024年第6期44卷 2994-3003页

作者：齐超楠齐鹏张艺铃北京工业大学环境与能源工程学院区域大气复合污染防治北京市重点实验室北京100124

通过实时高分辨率在线监测2019年邯郸市城区PM_(2.5)中碳组分和水溶性无机离子的质量浓度,分析研究了2019年全年邯郸市PM_(2.5)组分的变化特征和不同污染情景下PM_(2.5)组分的变化规律,同时采用正定矩阵因子分解模型和后向轨迹模型探究... 详细信息

通过实时高分辨率在线监测2019年邯郸市城区PM_(2.5)中碳组分和水溶性无机离子的质量浓度,分析研究了2019年全年邯郸市PM_(2.5)组分的变化特征和不同污染情景下PM_(2.5)组分的变化规律,同时采用正定矩阵因子分解模型和后向轨迹模型探究了PM_(2.5)及其组分的来源.结果表明:研究期间邯郸市PM_(2.5)中OC和EC的月变化和日变化特征相似.水溶性无机离子的季节变化特征为冬季>秋季>春季>夏季,NO_(3)-、SO_(4)^(2-)和NH_(4)^(+)是PM_(2.5)中主要的水溶性无机离子组分,在四个季节均与PM_(2.5)有较强的相关性.邯郸市PM_(2.5)呈弱碱性,NH4+主要以(NH_(4))_(2)SO_(4)、NH_(4)NO_(3)和NH_(4)Cl的形式存在.OC、EC和二次无机离子在PM_(2.5)污染日和O_(3)污染日有所增加.冬季污染加重时,碳组分和水溶性离子质量浓度随PM_(2.5)的增加而升高,OC和EC占比下降,SO_(4)^(2-)和NO_(3)-占比升高,且SOR和NOR也逐渐增加.PMF分析结果表明二次源,机动车源和燃烧源是邯郸市大气颗粒物污染的主要来源.后向轨迹结果表明邯郸市主要受到河南北部,山东西北部,山西中部和河北南部传输影响.该研究将会为重工业城市大气污染防治提供重要的科学理论依据.

关键词： PM_(2.5) 碳组分水溶性无机离子污染特征来源解析

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A Z/E isomeric cation designed organic-inorganic cadmium chloride ferroelectric with broadband white-light emission

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Science China Chemistry 2024年

作者： Jun-chao qi Yan qin Hang Peng Hui-Peng Lv Yong-Ju Bai Xin Shen Zhang-Tian Xia Wei-qiang Liao Ordered Matter Science Research Center Nanchang University

Hybrid organic-inorganic metal halides（HOMHs） have attracted tremendous interest in the past decades due to their diverse functional properties, such as ferroelectricity and luminescence. However, although a large number of ferroelectric HOMHs and luminescent HOMHs have been reported, the HOMH ferroelectrics with white-light emission remain very sparse. Here, for the first time, by using the Z/E isomeric organic cation, we designed a cadmium-based HOMH ferroelectric [EE-PMU]CdCl4（EEPMU = pyridin-2-ylmethanamide muconate） with broadband white-light emission. In contrast to the [ZZ-PMU]CdCl4with centrosymmetric crystal structure at room temperature, [EE-PMU]CdCl4adopts the polar crystal symmetry, which shows piezoelectricity with a piezoelectric coefficient of d33up to 19 pC/N and ferroelectricity with the saturated polarization of 1.52μC/cm2. Moreover, [EE-PMU]CdCl4exhibits a broadband white-light emission with an ultra-high color rendering index of 91 under UV excitation, which is related to the severely distorted [CdCl4]2-tetrahedron in the structure. To our knowledge, [EEPMU]CdCl4is the first example of Z/E isomeric cation-designed HOMH ferroelectric and the first cadmium halide white-light emissive ferroelectric. This finding paves a new way for the design of organic-inorganic molecular ferroelectrics with white-light emission.

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