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Highly N/O co-doped ultramicroporous carbons derived from nonporous metal-organic framework for high performance supercapacitors

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Chinese chemical Letters 2021年第4期32卷 1491-1496页

作者： Yangyi Gu Ling Miao Ying Yin Mingxian Liu Lihua Gan Liangchun Li shanghai key lab of chemical assessment and sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China

A new nonporous Zn-based metal-organic framework(NPMOF) synthesized from a high nitrogencontaining rigid ligand was converted into porous carbon materials by direct carbonization without adding additional carbon sources.A series of NPMOF-derived porous carbons with very high N/O contents(24.1% for NPMOF-700,20.2% for NPMOF-800,15.1% for NPMOF-900) were prepared by adjusting the pyrolysis *** NPMOF-800 fabrica ted electrode exhibits a high capacitance of220 F/g and extremely large surface area normalized capacitance of 57.7 μF/cm~2 compared to other reported MOF-derived porous carbon electrodes,which could be attributed to the abundant ultramicroporosity and high N/O *** importantly,symmetric supercapacitor assembled with the MOF-derived carbon manifests prominent stability,i.e.,99.1 % capacitance retention after 10,000 cycles at 1.0 A/*** simple preparation of MOF-derived porous carbon materials not only finds an application direction for a variety of porous or even nonporous MOFs,but also opens a way for the production of porous carbon materials for superior energy storage.

关键词： N/O co-doped Ultramicroporous Metal-organic frameworks Porous carbons Supercapacitors

A general strategy via photoelectrocatalytic oxygen reduction for generating singlet oxygen with carbon bridged carbon-nitride electrode

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Chinese chemical Letters 2021年第11期32卷 3393-3397页

作者： Qianqian Yang Zhiyuan Feng Mingyue Liu Jinxing Zhang Hongying Zhao Guohua Zhao School of chemical Science and Engineering and Shanghai Key Lab of Chemical Assessment and SustainabilityTongji UniversityShanghai 200092China

With the ever-growing demand of clean water for the healthy world,water purification has become an urgent global *** oxygen(^(1)O_(2))as unique non-radical derivative of oxygen,possessing unoccupiedπ*orbital and exhibiting high selectivity towards electron-rich organic ***,most of the approaches suffer from low-efficiency or biotoxicity,which severely restrict their potential ***,in this work,we propose a general strategy via photoelectrocatalytic for selectively reducing oxygen to^(1)O_(2)with designed carbon bridged carbon nitride(CBCN).This work highlights the important role of synergistic photo-electro-catalytic effect for selectively generating the^(1)O_(2)via oxygen reduction pathway,which can be a promising way especially for degrading electron-rich pollutants.

关键词： Oxygen reduction reaction Singlet oxygen Photoelectrocatalytic process Carbon-nitride Wastewater treatment

Synthesis of chiral allylic phosphonates via asymmetric reductive cross-coupling of α-bromophosphonates and vinyl bromides

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Science China Chemistry 2023年第9期66卷 2621-2625页

作者： Hepan Wang Xinxuan Li Tao XU shanghai key laboratory of chemical assessment and sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China

Chiral phosphine-containing skeletons play a pivotal role in bioactive natural products, pharmaceuticals, chiral catalysts, and ligands. Despite considerable progress has been made in the synthesis of chiral phosphorus compounds, the development of facile and modular methods to access chiral allylic phosphorus compounds remains challenging due to the simultaneous control required for reactivity, enantioselectivity, and stereoselectivity. Herein, we present a general and modular platform to achieve the asymmetric reductive cross-coupling of α-bromophosphonates and vinyl bromides, enabling the synthesis of highly valuable chiral allylic phosphonate products with remarkable yields, enantioselectivities, and stereoselectivities.

关键词： chiral phosphorus compound reductive cross-coupling α-alkenyl phosphonate nickel asymmetric reaction

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Expediting H_(2)Evolution over MAPbI_(3)with a Nonnoble Metal Cocatalyst Mo_(2)C under Visible Light

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Energy Material Advances 2022年第1期2022卷 231-240页

作者： Jinxing Yu Xiaoxiang Xu shanghai key lab of chemical assessment and sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China

Halide perovskites have been emerging as promising photocatalytic materials for H_(2)evolution from water due to their outstanding photoelectric ***,the lack of proper surface reactive sites greatly hinders the photocatalytic potential of these fascinating ***,Mo_(2)C nanoparticles have been anchored onto methylammonium lead iodide(MAPbI_(3))as a nonnoble metal cocatalyst to promote H_(2)evolution *** Mo_(2)C nanoparticles have opposite zeta potential with MAPbI_(3)thereby electrostatically assembled onto the MAPbI_(3)surface,i.e.,Mo_(2)C@MAPbI_(3).Our results show that the anchored Mo_(2)C nanoparticles have a strong interplay with MAPbI_(3)substrate so that photogenerated electrons of MAPbI_(3)can be rapidly separated and transferred into Mo_(2)C for further H_(2)evolution *** optimal conditions,Mo_(2)C@MAPbI_(3)delivers exceptionally high photocatalytic performance for visible light-driven H_(2)evolution that clearly outperforms pristine MAPbI_(3)and Pt-deposited MAPbI_(3).An apparent quantum efficiency as high as 12.65%at 600±40 nm has been attained for H_(2)evolution,surpassing most of the MAPbI_(3)-based photocatalyst *** results signify the usefulness and applicability of Mo_(2)C as a new nonnoble metal-based cocatalyst in solar water splitting.

关键词： catalyst noble thereby

A Self-supported Graphene/Carbon Nanotube Hollow Fiber for Integrated Energy Conversion and Storage

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Nano-Micro Letters 2020年第5期12卷 95-105页

作者： Kai Liu Zilin Chen Tian Lv Yao Yao Ning Li Huili Li Tao Chen shanghai key lab of chemical assessment and sustainability School of Chemical Science and Engineeringand Institute of Advanced StudyTongji UniversityShanghai 200092People’s Republic of China

Wearable fiber-shaped integrated energy conversion and storage devices have attracted increasing attention,but it remains a big challenge to achieve a common fiber electrode for both energy conversion and storage with high ***,we grow aligned carbon nanotubes(CNTs)array on continuous graphene(G)tube,and their seamlessly connected structure provides the obtained G/CNTs composite fiber with a unique self-supported hollow *** advantage of the hollow structure,other active materials(e.g.,polyaniline,PANI)could be easily functionalized on both inner and outer surfaces of the tube,and the obtained G/CNTs/PANI composite hollow fibers achieve a high mass loading(90%)of *** G/CNTs/PANI composite hollow fibers can not only be used for high-performance fiber-shaped supercapacitor with large specific capacitance of 472 mF cm^-2,but also can replace platinum wire to build fiber-shaped dye-sensitized solar cell(DSSC)with a high power conversion efficiency of 4.20%.As desired,the integrated device of DSSC and supercapacitor with the G/CNTs/PANI composite hollow fiber used as the common electrode exhibits a total power conversion and storage efficiency as high as 2.1%.Furthermore,the self-supported G/CNTs hollow fiber could be further functionalized with other active materials for building other flexible and wearable electronics.

关键词： Carbon nanotube Graphene Integrated Energy conversion Energy storage

Ta_(3)N_(5)–LaTaON_(2) heterojunction with matched interfaces to accelerate charge separation for efficient photocatalytic water oxidation

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Journal of Materials Science & Technology 2023年第23期154卷 241-250页

作者： Guoan Lin Chi Zhang Xiaoxiang Xu Clinical and Central lab Putuo People's Hospital Tongji University Shanghai 200060 China shanghai key lab of chemical assessment and sustainability School of Chemical Science and Engineering Tongji University Shanghai 200092 China

Charge separation is generally considered as the most critical step to achieve efficient photocatalytic reactions. Although charge separation can be promoted by a semiconductor heterojunction, its efficacy is inherently restrained by the mismatched atomic arrangements across the heterojunction interfaces. Here, Ta3N5–LaTaON2 heterojunction with matched interfaces has been fabricated by one-step ammonolysis treatment of KLaTa2O7. The match interfaces are formed by nearly perfect adhesion of Ta3N5 (010) and LaTaON2 (101¯) facets whose interatomic distance is similar. Compared with conventional heterojunction, the so-formed Ta3N5–LaTaON2 heterojunction are extremely efficient in accelerating charge separation which in turn enables a high photocatalytic activity. An apparent quantum efficiency as high as 11.6% at 420 ± 20 nm has been reached by Ta_(3)N_(5)–LaTaON_(2) heterojunction, which is almost three times higher than Ta_(3)N_(5)-LaTaON_(2) mixtures. These results signify the importance of matched heterojunction interfaces for charge separation and provide a paradigm in the design of efficient heterojunction-based semiconductor photocatalysts.

关键词： Semiconductor heterojunction LaTaON_(2) Ta_(3)N_(5) Photocatalyst Water oxidation

Nanotechnologies for enhancing cancer immunotherapy

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Nano Research 2020年第10期13卷 2595-2616页

作者： Jingxian Yang Chunhui Wang Shuo Shi Chunyan Dong Breast cancer center Shanghai East HospitalSchool of MedicineShanghai Key Laboratory of Chemical Assessment and SustainabilitySchool of Chemical Science and EngineeringTongji UniversityShanghai 200120China

Immunotherapy,a burgeoning field differs from traditional cancer treatments,is revolutionizing oncologic *** aims to stimulate the innate and adaptive immune system of a patient to fight against tumor ***,low response rate and immune-related adverse effects(irAEs)remain problems during its management.A novel technology using nanomaterials may bring a *** nanoparticles have been investigated as delivery systems to augment cancer therapeutic efficacy in the lab and *** this review,we briefly summarize the connotation of immunotherapy,the application of nanotechnology in cancer,especially focusing on the synergistic effect of nanoplatform-based technology combined with cancer immunotherapy,hoping to make readers a deep insight into this interdisciplinary field.

关键词： cancer im munotherapy nanoplatform-based technology combination therapy synergistic effect

Magnetically separated and N, S co-doped mesoporous carbon microspheres for the removal of mercury ions

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Chinese chemical Letters 2016年第5期27卷 795-800页

作者： Ming-Xian Liu Xiang-Xiang Deng Da-Zhang Zhu Hui Duan Wei Xiong Zi-Jie Xu Li-Hua Gan shanghai key lab of chemical assessment and sustainability Department of Chemistry Tongji University School of Chemistry and Environmental Engineering Wuhan Institute of Technology

Magnetically separated and N, S co-doped mesoporous carbon microspheres （NIS-MCMs/Fe304） are fabricated by encapsulating Si02 nanoparticles within N, S-containing polymer microspheres which were prepared using resorcinol/formaldehyde as the carbon source and cysteine as the nitrogen and sulfur co-precursors, followed by the carbonization process, silica template removal, and the introduction of Fe3O4 into the carbon mesopores. N/S-MCMs/Fe3O4 exhibits an enhanced Hg2＋ adsorption capacity of 74.5 rag/g, and the adsorbent can be conveniently and rapidly separated from wastewater using an external magnetic field. This study opens up new opportunities to synthesize well- developed, carbon-based materials as an adsorbent for potential applications in the removal of mercury ions from wastewater.

关键词： N S co-doped mesoporous carbonmicrospheres MagnetiteAdsorption Mercury ion Magnetic separation

Zinc tartrate oriented hydrothermal synthesis of microporous carbons for high performance supercapacitor electrodes

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Chinese chemical Letters 2016年第3期27卷 399-404页

作者： Ming-Xian Liu Ling-Yan Chen Da-Zhang Zhu Hui Duan Wei Xiong Zi-Jie Xu Li-Hua Gan Long-Wu Chen shanghai key lab of chemical assessment and sustainability Department of ChemistryTongji University School of Chemistry and Environmental Engineering Wuhan Institute of Technology

A novel zinc tartrate oriented hydrothermal synthesis of microporous carbons was reported. Zinc–organic complex obtained via a simple chelation reaction of zinc ions and tartaric acid is introduced into the networks of resorcinol/formaldehyde polymer under hydrothermal condition. After carbonization process, the resultant microporous carbons achieve high surface area（up to 1255 m^2/g） and large mean pore size（1.99 nm） which guarantee both high specific capacitance（225 F/g at 1.0 A/g） and fast charge/discharge operation（20 A/g） when used as a supercapacitor electrode. Besides, the carbon electrode shows good cycling stability, with 93% capacitance retention at 1.0 A/g after 1000 cycles. The welldesigned and high-performance microporous carbons provide important prospects for supercapacitor applications.

关键词： Zinc tartrate Hydrothermal synthesis Microporous carbon Supercapacitor Electrode