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Chinese Journal of chemistry 2024年第6期42卷 617-622页

作者： Wei-Xing Chen Yu-He Xu Cui-Cui Wang Lei Qiao Zi-yan Guo Wen-Juan Tian Zhong-Ming Sun state key laboratory of Element-Organic chemistry Tianjin Key Lab for Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin300350 China Institute of Molecular Science Shanxi UniversityTaiyuanShanxi030006 China

Binary polyantimony clusters,namely[Cu_(2)Sb_(14)]^(4–) and [Ag_(2)Sb_(14)]^(4–),containing coinage metals,were successfully synthesized and characterized,in which two homoatomic Sb73–subunits are bridged by two coinage metals in η^(4):η^(1) and η^(1):η^(1) coordination modes,***[M_(2)Sb_(14)]^(4-),two bridging Cu ions and two Sb atoms form a planar rhombic unit,which was revealed to have antiaromatic properties by theoretical *** electron structure and bonding analysis confirmed the presence of delocalized bonds in the rhombic unit and the metallophilic interaction between two formal M^(+) ions.

关键词： Polyantimony cluster Copper Silver Antiaromaticity Metallophilic interaction Quantum chemical calculations

Metal-encapsulated nitrogen-doped carbon nanotube arrays electrode for enhancing sulfion oxidation reaction and hydrogen evolution reaction by regulating of intermediate adsorption

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Chinese chemical Letters 2024年第8期35卷 533-538页

作者： Xiao Li Wanqiang Yu Yujie Wang Ruiying Liu Qingquan Yu Riming Hu Xuchuan Jiang Qingsheng Gao hong Liu Jiayuan Yu Weijia Zhou Institute for Advanced Interdisciplinary Research(iAIR) School of Chemistry and Chemical EngineeringUniversity of JinanJi’nan 250022China Institute for Smart Materials&engineering School of Materials Science and EngineeringUniversity of JinanJi’nan 250022China College of chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China state key laboratory of Crystal Materials Shandong UniversityJi’nan 250100China

For treatment of sulfion-containing wastewater,coupling the electrochemical sulfion oxidation reaction(SOR)with hydrogen evolution reaction(HER)can be an ideal way for sulfur and H_(2)resources ***,we synthesize a metal-modified carbon nanotube arrays electrode(Co@N-CNTs/CC)for SOR and *** electrode has excellent performance for SOR and HER attributed to the unique array *** can achieve 99.36 mA/cm^(2)at 0.6 V for SOR,and 10 mA/cm^(2)at 0.067 V for *** functional theory calculations verify that metal modification is able to regulate the electronic structure of carbon nanotube,which is able to optimize the adsorption of *** Co@N-CNTs/CC as bifunctional elec-trodes to establish a hybrid electrolytic cell can reduce about 67%of energy consumption compared with the traditional water splitting electrolytic ***,the hybrid electrolytic cell is used to treat actual sulfion-containing wastewater,achieving the sulfur yield of 30 mg h^(−1)cm^(−2)and the hydrogen production of 0.64 mL/min.

关键词： Sulfion oxidation reaction Hydrogen evolution reaction Nitrogen-doping carbon nanotube Core-shell structure Resource upgrade

The proximity between hydroxyl and single atom determines the catalytic reactivity of Rh1/CeO_(2) single-atom catalysts

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Nano Research 2024年第1期17卷 397-406页

作者： Danfeng Wu Shuyun Zhou Congcong Du Juan Li Jianyu Huang hong-xia Shen Abhaya K.Datye Shan Jiang Jeffrey T.Miller Sen Lin Haifeng Xiong state key laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state key laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhou 350002China Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004China College of Biology and chemical engineering Jiaxing UniversityJiaxing 314000China Department of chemical&Biological engineering University of New MexicoAlbuquerqueNM 8731-0001USA Davidson school of chemical engineering Purdue UniversityWest LafayetteIN 47907-2100USA Innovation laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China Fujian key laboratory of Rare-earth Functional Materials Fujian Shanhai Collaborative Innovation Center of Rare-earth Functional MaterialsLongyan 366300China

The local structure of the metal single-atom site is closely related to the catalytic activity of metal single-atom catalysts(SACs).However,constructing SACs with homogeneous metal active sites is a challenge due to the surface heterogeneity of the conventional ***,we prepared two Rh1/CeO_(2)SACs(0.5Rh1/r-CeO_(2)and 0.5Rh1/c-CeO_(2),respectively)using two shaped CeO_(2)(rod and cube)exposing different facets,i.e.,CeO_(2)(111)and CeO_(2)(100).In CO oxidation reaction,the T100 of 0.5Rh1/r-CeO_(2)SACs is 120°C,while the T100 of 0.5Rh1/c-CeO_(2)SACs is as high as 200°*** in-situ CO diffuse reflectance infrared Fourier transform spectroscopy(CO-DRIFTS),we found that the proximity between OH group and Rh single atom on the plane surface plays an important role in the catalytic activity of Rh1/CeO_(2)SAC system in CO *** Rh single atom trapped at the CeO_(2)(111)crystal surface forms the Rh1(OH)adjacent species,which is not found on the CeO_(2)(100)crystal surface at room ***,during CO oxidation,the OH group far from Rh single atom on the 0.5Rh1/c-CeO_(2)disappears and forms Rh1(OH)adjacent species when the temperature is above 150°*** formation of Rh1(OH)adjacentCO intermediate in the reaction is pivotal for the excellent catalytic activity,which explains the difference in the catalytic activity of Rh single atoms on two different CeO_(2)*** formed Rh1(OH)adjacent-O-Ce structure exhibits good stability in the reducing atmosphere,maintaining the Rh atomic dispersion after CO oxidation even when pre-reduced at high temperature of 500°*** functional theory(DFT)calculations validate the unique activity and reaction path of the intermediate Rh1(OH)adjacentCO species *** work demonstrates that the proximity between metal single atom and hydroxyl can determine the formation of active intermediates to affect the catalytic performances in catalysis.

关键词： crystal plane Rh1/CeO_(2)single-atom catalyst proximity of Rh and hydroxyl coordination structure CO oxidation

H_(2)O_(2)辅助污泥水热过程水DOM的光化学行为研究

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中国环境科学 2024年第6期44卷 3179-3188页

作者：张闯王冰玉谢慧芳冯彦房曲虹霞南京理工大学环境与生物工程学院化工污染控制与资源化江苏省高校重点实验室江苏南京210094 江苏省农业科学院农业资源与环境研究所农业农村部长江下游平原农业环境重点实验室江苏南京210014 南京理工大学化学与化工学院江苏南京210094

采用水热炭化和添加4%H_(2)O_(2)辅助水热炭化两种工艺处理脱水污泥,在测定两种过程水DOM基本理化性质的基础上,重点比较了两种DOM的光漂白行为和光生活性物种的产生情况.结果表明,与水热炭化工艺相比,H_(2)O_(2)辅助水热炭化工艺中伴... 详细信息

采用水热炭化和添加4%H_(2)O_(2)辅助水热炭化两种工艺处理脱水污泥,在测定两种过程水DOM基本理化性质的基础上,重点比较了两种DOM的光漂白行为和光生活性物种的产生情况.结果表明,与水热炭化工艺相比,H_(2)O_(2)辅助水热炭化工艺中伴生的过程水DOM的pH值较低,电导率、TOC、腐殖质类物质含量、芳香性官能团、分子量及腐殖化程度均较高,并表现出更强的光敏感性.在模拟自然光照射条件下,其芳香性和腐殖化程度随光照时间延长而降低,荧光组分含量显著下降,其中腐殖质类组分降低最为明显.光照过程中产生更多的单线态氧(1O2)和三重激发态(^(3)DOM^(*)),可显著促进四环素的光降解(93.22%),且^(3)DOM^(*)起主导作用.本研究明确了H_(2)O_(2)辅助水热炭化过程水DOM的光化学行为,可为水热炭化处理污泥产生的过程水的进一步处理及利用提供理论依据.

关键词：辅助水热炭化溶解性有机质(DOM) 光漂白光降解四环素

Structural parameterization and functional prediction of antigenic polypeptome sequences with biological activity through quantitative sequence-activity models (QSAM) by molecular electronegativity edge-distance vector (VMED)

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Science china(Life Sciences) 2007年第5期50卷 706-716页

作者： LI ZhiLiang1,2, WU ShiRong1,2, CHEN ZeCong1,2, YE Nancy1,2, yanG ShengXi1,2, LIAO Chunyang1,2, ZHANG MengJun1,2,3, yanG Li1,2, MEI Hu1,2,4, yanG yan1,2, ZHAO Na1,2, ZHOU Yuan1,2, ZHOU Ping1,2, XIONG Qing1,2, XU hong1,2, LIU ShuShen1,2, LING ZiHua1,2, CHEN Gang1,2,4 & LI GenRong1,2 1 College of chemistry and chemical engineering/key laboratory for Chemobiomedical Science and engineering under Chongqing Municipality, College of Life Science and Biological engineering/key laboratory for Biomechanics and Tissue engineering under Ministry of Education, Chongqing university, Chongqing 400044, china 2 state key laboratory for Chemobiosensors and Chemobiometrics under MOST at Hunan university, Changsha 410012, china 3 Department of Medical Analysis/PLA Center of Bioinformatics Immunology, Surgeon Third university, Chongqing 400031, china 4 Technology Centre for Life Sciences, Singapore Polytechnic, 500 Dover Road, Singapore 139651, Singapore 1. College of chemistry and chemical engineering/key laboratory for Chemobiomedical Science and engineering under Chongqing Municipality College of Life Science and Biological Engineering/Key Laboratory for Biomechanics and Tissue Engineering under Ministry of Education Chongqing University Chongqing 400044 China 2. state key laboratory for Chemobiosensors and Chemobiometrics under MOST at Hunan university Changsha 410012 China 3. Department of Medical Analysis/PLA Center of Bioinformatics Immunology Surgeon Third University Chongqing 400031 China 4. Technology Centre for Life Sciences Singapore Polytechnic 500 Dover Road Singapore 139651 Singapore

Only from the primary structures of peptides, a new set of descriptors called the molecular electro-negativity edge-distance vector (VMED) was proposed and applied to describing and characterizing the molecular structures of oligopeptides and polypeptides, based on the electronegativity of each atom or electronic charge index (ECI) of atomic clusters and the bonding distance between atom-pairs. Here, the molecular structures of antigenic polypeptides were well expressed in order to propose the auto-mated technique for the computerized identification of helper T lymphocyte (Th) epitopes. Furthermore, a modified MED vector was proposed from the primary structures of polypeptides, based on the ECI and the relative bonding distance of the fundamental skeleton groups. The side-chains of each amino acid were here treated as a pseudo-atom. The developed VMED was easy to calculate and able to work. Some quantitative model was established for 28 immunogenic or antigenic polypeptides (AGPP) with 14 (1― 14) Ad and 14 other restricted activities assigned as "1"(+) and "0"(-), respectively. The latter comprised 6 Ab(15-20), 3 Ak(21-23), 2 Ek(24-26), 2 H-2k(27 and 28) restricted sequences. Good results were obtained with 90% correct classification (only 2 wrong ones for 20 training samples) and 100% correct prediction(none wrong for 8 testing samples); while con-trastively 100% correct classification (none wrong for 20 training samples) and 88% correct classification (1 wrong for 8 testing samples). Both stochastic samplings and cross valida-tions were performed to demonstrate good performance. The described method may also be suitable for estimation and prediction of classes I and II for major histocompatibility an-tigen (MHC) epitope of human. It will be useful in immune identification and recognition of pro-teins and genes and in the design and devel-opment of subunit vaccines. Several quantitative structure activity relationship (QSAR) models were developed for various oligop

关键词： molecular electronegativity distance-edge vector (VMED), antigenic polypeptide (AGPP) sequences, bioactive oligopeptide (BAOP) chains, quantitative sequence-activity models (QSAM), theoretically computational descriptors (TCD)

胺源对“一锅法”合成聚硼硅氮烷结构及性能的影响

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高分子学报 2024年第2期55卷 161-171页

作者：陈楚童陈艳杰罗永明张宗波徐彩虹中国科学院化学研究所中国科学院极端环境高分子材料重点实验室北京100190 中国科学院大学化学与化工学院北京100049

以六甲基二硅氮烷(MMN)、四甲基二乙烯基二硅氮烷(MMNVi)和四甲基二硅氮烷(MMNH) 3种不同结构的二硅氮烷为胺源,通过与氯硅烷和三氯化硼反应,制备出具有不同封端结构的聚硼硅氮烷.其中,以MMN、MMNVi为胺源可获得液态产物;以MMNH为胺源时... 详细信息

以六甲基二硅氮烷(MMN)、四甲基二乙烯基二硅氮烷(MMNVi)和四甲基二硅氮烷(MMNH) 3种不同结构的二硅氮烷为胺源,通过与氯硅烷和三氯化硼反应,制备出具有不同封端结构的聚硼硅氮烷.其中,以MMN、MMNVi为胺源可获得液态产物;以MMNH为胺源时,因合成过程中发生活性基团间的过度交联导致产物凝胶.采用核磁共振波谱仪、红外光谱仪对液态前驱体聚合物及其热解产物的结构进行了表征.研究结果表明:通过“一锅法”制备的液态聚硼硅氮烷主链具有较多的支化和环状结构,随着封端结构中乙烯基含量的增加,所得前驱体的固化温度降低,固化反应活化能降低.与以MMN为胺源和封端剂合成的聚硼硅氮烷相比,以MMNVi为胺源所得前驱体固化前后陶瓷产率分别提高了14.9%及8.1%.并且,通过改变胺源的种类和比例可以调节热解产物的元素组成,合成的液态前驱体聚合物热解所得SiBCN陶瓷结晶温度高于1700℃.

关键词：前驱体转化法硅硼碳氮陶瓷聚硼硅氮烷 “一锅法”

Toluene Processed All-Polymer Solar Cells with 18% Efficiency and Enhanced Stability Enabled by Solid Additive:Comparison Between Sequential-Processing and Blend-Casting

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Energy & Environmental Materials 2024年第4期7卷 247-254页

作者： Guoping Zhang Chaoyue Zhao Liangxiang Zhu Lihong Wang Wenzhao Xiong Huawei Hu Qing Bai Yaping Wang Chen Xie Peng You He yan Dan Wu Tao yang Mingxia Qiu Shunpu Li Guangye Zhang College of New Materials and New Energies Shenzhen Technology University Department of chemistry and hong Kong Branch of Chinese National engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and Technology state key laboratory for Modification of chemical Fibers and Polymer Materials Center for Advanced Low-dimension Materials College of Materials Science and Engineering Donghua University Julong College Shenzhen Technology University

The emergence of polymerized small molecule acceptors (PSMAs) has significantly improved the performance of all-polymer solar cells (all-PSCs).However,the pace of device engineering lacks behind that of materials deve... 详细信息

关键词： all-polymers solar cells sequential processing solid additive

馄饨结构的KB@Co-C_(3)N_(4)在中性电解质中作为锌空气电池的高活性和稳定性氧催化剂

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Chinese Journal of Catalysis 2024年第5期60卷 178-189页

作者：吴维凡范晋歌赵振宏潘建敏杨静阎兴斌詹怡中山大学化学工程与技术学院广东珠海519082 中山大学低碳化学与节能工程重点实验室广东广州510275 中山大学材料科学与工程学院光电材料与技术国家重点实验室广东广州510275

金属和氮共掺杂碳(M-N-Cs)由于具有高原子利用率、良好的活性和选择性,因而被认为是具有潜力的氧电催化剂.但其热力学氧化势较低,碳材料在高电位下容易腐蚀.在放电过程中,锌空气电池正极的电位始终比碳氧化的热力学电位高约0.5 V,这导... 详细信息

金属和氮共掺杂碳(M-N-Cs)由于具有高原子利用率、良好的活性和选择性,因而被认为是具有潜力的氧电催化剂.但其热力学氧化势较低,碳材料在高电位下容易腐蚀.在放电过程中,锌空气电池正极的电位始终比碳氧化的热力学电位高约0.5 V,这导致阴极中碳的严重腐蚀.对于M-N-C,腐蚀会破坏金属氮配位(M-Nx)活性位点,导致活性比表面积减少,同时还会改变孔隙形貌和表面特性,进而降低其催化活性.在充电(即氧气析出反应,OER)过程中,这种腐蚀现象会进一步加剧.因此,开发一种既具有高效双功能催化活性,又具有良好抗电化学腐蚀性能的M-N-C催化剂,对于解决上述问题至关重要.本文利用氮化碳(g-C_(3)N_(4))支撑钴氮配位(Co-Nx)活性位点,同时包覆科琴黑(KB)形成馄饨结构,制备了双功能氧催化剂KB@Co-C_(3)N_(4).首先,将剥离的C_(3)N_(4)与KB混合后煅烧,得到C_(3)N_(4)包覆的KB材料(KB@C_(3)N_(4));随后,再次煅烧将Co单原子引入KB@C_(3)N_(4)中,形成具有高活性和高稳定性的KB@Co-C_(3)N_(4)氧催化剂.红外光谱结果证实了,KB@Co-C_(3)N_(4)中存在C_(3)N_(4)成分.透射电镜和元素标记结果表明,C_(3)N_(4)均匀包覆在KB基底上.同步辐射测试确定了Co单原子的配位环境为CoN4结构.在0.5 mol L^(-1) NH_(4)Cl溶液中测试了KB@Co-C_(3)N_(4)氧催化剂ORR/OER的催化活性和稳定性.结果表明,KB@CoC_(3)N_(4)表现出较好的ORR性能,半波电位为0.723 V,显著优于商业铂碳催化剂(0.673 V)和普通Co-N-C催化剂(0.694 V).经过40000圈加速耐久性测试,KB@Co-C_(3)N_(4)仅衰减9 mV,而商业铂碳和Co-N-C在7500圈测试后分别衰减41和44 mV.在OER方面,KB@Co-C_(3)N_(4)在10 mA cm^(-2)时的过电位为550 mV,优于氧化钌的560 mV和Co-N-C的600 mV.经过20000圈测试,KB@Co-C_(3)N_(4)的OER过电位几乎保持不变,而氧化钌和Co-N-C经过4000圈测试后分别增加了37和20 mV.透射电镜观察发现,KB@Co-C_(3)N_(4)在实验前后形貌未发生明显变化,证明了其较好的稳定性.理论计算揭示,C_(3)N_(4)能够优化Co金属活性位点的电子结构,改善Co中心的电荷分布并增强Co-N键强度;同时,C_(3)N_(4)对KB基底的包覆有效避免了KB在高电位下的腐蚀,确保了KB@Co-C_(3)N_(4)的高稳定性和催化活性.将KB@Co-C_(3)N_(4)应用于中性锌空气电池中,该电池展现出1.52 V的开路电压,并在5 mA cm^(-2)的高电流密度下稳定循环运行超过985 h,性能优于大多数报道的采用碳基材料作为阴极催化剂的中性锌空气电池.综上所述,馄饨结构的KB@Co-C_(3)N_(4)具有较好的氧催化活性和稳定性,为设计高稳定性高活性的M-N-C催化剂提供了一定的参考.

关键词：氧电催化单原子催化剂中性电解液抗腐蚀

Efficient and stable organic solar cells enabled by a poly(carbazole phosphonic acid)hole transporter

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Science china chemistry 2024年第6期67卷 1941-1945页

作者： Zhijun Ren Siwei Luo Xiaoyu Shi Yunjie Dou Tianxiao Liu Lingyuan Wang Kwok Kiu Tsang Feifei Wang Yu Zhao yangyang Liu Xiaodong Hu Xiaoxiao Peng Wei Liu He yan Shangshang Chen state key laboratory of coordination chemistry MOE Key Laboratory of High Performance Polymer Materials&TechnologySchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing210023China Department of chemistry Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional MaterialsEnergy Institute and Hong Kong Branch of Chinese NationalEngineering Research Center for Tissue Restoration and ReconstructionHong Kong University of Science and TechnologyHong Kong999077China

Conventional self-assembled monolayer(SAM)hole transporters in organic solar cells(OSCs)generally suffer from poor uniformity and limited thickness tolerance,hindering their large-scale *** overcome these limitations,we introduce a novel polymeric hole transporter synthesized by polymerizing carbazole phosphonic acid(PACz).The resultant Poly-2PACz material exhibits exceptional conductivity,high tolerance for variations in layer thickness,and improved film uniformity compared with conventional ***,the OSCs utilizing Poly-2PACz achieve a remarkable power conversion efficiency of 19.1%and a high fill factor of 81.2%,surpassing the devices based on ***,Poly-2PACz-based OSCs demonstrate excellent operational stability,retaining over 80%of their initial efficiency after 1,400 h of continuous light exposure in ambient *** work presents a novel strategy for designing hole transporters,paving the way for more efficient and stable OSCs.

关键词： organic solar cells hole transporters poly(carbazole phosphonic acid) stability

Review for chiral-at-metal complexes and metal-organic framework enantiomorphs

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Science Bulletin 2017年第19期62卷 1344-1354页

作者： Zi-hong yan Donghao Li Xue-Bo Yin College of chemistry and Environmental Sciences Laboratory of Xinjiang Native Medicinal and Edible Plant Resources ChemistryKashgar University key laboratory of Natural Resource of the Changbai Mountain and Functional Molecular Ministry of EducationYanbian University state key laboratory of Medicinal chemical Biology and Tianjin key laboratory of Biosensing and Molecular Recognition College of ChemistryNankai University

This review discusses chiral-at-metal complexes and introduces enantiomorphs from assembly *** to the diverse coordination number and activity of metal ions as chiral centers, abundant structures for chiral selectivity, catalysis, and polarized light-response are the notable advantages of the chiral-at-metal complexes. The rational design and preparation of linear multi-dentate ligands is a good choice to improve the stability of chiral complexes, such as multi-bonding structure for high stability as a self-limiting system. The bio-significance and potential application of chiral-at-metal complexes are discussed, such as the synergistic effect of catalysis and chiral selectivity of the metal center in *** could be remolded to replace the original central metal ions with highly active rare earth or precious metal ions to form artificial metalloenzyme or to remove the ‘‘redundant" part around the metal center to improve the accessibility of substrate. The polarized light-response mechanism of chiral opsin is introduced in relation to its role in animal migration. Metal-organic frameworks(MOFs) are crystalline and porous materials built from metal nodes or clusters and organic linkers and provide the possibility to prepare artificial enantiomorphs. The preparations, applications, and characterization methods of MOF enatiomorphs are therefore introduced. We hope this review inspires researchers at all levels of their career to consider the title topic in their own research in terms of its application and potential value.

关键词： ChiralityStereoisomerChiral-at-metal complexAssembly enatiomorphChiral metal-organic frameworks