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Chinese Chemical Letters 2023年第2期34卷 224-229页

作者： Yige Deng Song Shu Ningjie Fang Ruobing Wang Yinghao Chu Zhaobing Liu wanglai cen College of Architecture and Environment Sichuan UniversityChengdu 610065China Chengdu Environment Group Chengdu 610065China Institute of New Energy and Low Carbon Technology Sichuan UniversityChengdu 610065China

Photocatalytic hydrogen evolution from water splitting is a promising strategy for realizing the vision of carbon neutrality.Herein,a novel SrTi O_(3)-SrCO_(3)n-n heterojunction was used for the first time for water splitting to generate H_(2).The heterojunction was synthesized by a soft chemical one-pot hydrothermal method.The Sr TiO_(3)-SrCO_(3)loading with 3 wt%Pt shows the maximum photocatalytic H_(2)evolution rate of3.62 mmol h^(-1)g^(-1)under simulated sunlight irradiation,which is 20.1 times higher than that of pristine SrTiO_(3).The apparent quantum efficiency of Sr TiO_(3)-SrCO_(3)reaches 21.73%at 313 nm,and it shows good stability during cyclic experiment.The formation of compact Sr TiO_(3)-SrCO_(3)heterojunction with strong interfacial electronic interaction promotes the transmission and separation of photo-generated carriers.The results of XPS,PL,PC,EIS and DFT support the mechanism of improving photocatalytic activity based on carrier dynamics.This work provides a facile and effective method to enhance the activity of Sr Ti O_(3)-based heterojunction photocatalysts.

关键词： SrTiO_(3)/SrCO_(3) Heterojunction Photocatalytic Hydrogen evolution Nanomaterial

Flash-assisted doping graphene for ultrafast potassium transport

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Nano Research 2022年第5期15卷 4083-4090页

作者： Yongzhi Zhang Xianjue Chen wanglai cen Wenhao Ren Haocheng Guo Sicheng Wu Yang Xiao Sheng Chen Yong Guo Dan Xiao Chuan Zhao Institute of New Energy and Low-Carbon Technology(INELT) Sichuan UniversityChengdu 610065China School of Chemistry University of New South WalesSydney 2052Australia College of Chemistry Sichuan UniversityChengdu 610064China

Graphene has been widely used for electrical energy storage and its performances could be further improved by heteroatom doping.How to prepare doped graphene efficiently and economically remains a significant challenge.Here,we propose a flash-assisted doping method to produce nitrogen-and sulfur-doped graphene(N-rGO and S-rGO).Using this method,graphene oxide(GO)is reduced to few-layer graphene(rGO)in seconds without the use of reductants,accompanied with a high doping efficiency.Particularly,the as-synthesized N-rGO with a high N content of 12.75 at.%used as potassium-ion battery(KIB)anode exhibits ultrafast K+-transport kinetics and superior K^(+)-storage capability.Quantitative kinetics analysis and theoretical simulation are used to reveal the mechanism of transportation and storage of K^(+)in N-rGO.

关键词： graphene doping flash anodes potassium-ionbatteries

An upgraded polymeric composite with interparticle chemical bonding microstructure toward lithium-ion battery separators with enhanced safety and electrochemical performances

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能源化学:英文版 2023年第9期84卷 402-413页

作者： Qian Zhao Ling Ma Ye Xu Xiulong Wu Shuai Jiang Qiaotian Zheng Guang Hong Bin He Chen Li wanglai cen Wenjun Zhou Yan Meng Dan Xiao College of Mechanical Engineering Chengdu UniversityChengdu 610106SichuanChina Institute for Advanced Study Chengdu UniversityChengdu 610106SichuanChina Chongqing Academy of Metrology and Quality Inspection Chongqing 401121China Institute of New Energy and Low-Carbon Technology Sichuan UniversityChengdu 610065SichuanChina

A composite separator of SiC/PVDF-HFP was synthesized for lithium-ion batteries with high thermal and mechanical stabilities.Benefiting from the nanoscale,high hardness,and melting point of SiC,SiC/PVDFHFP with highly uniform microstructure was obtained.This polarization caused by barrier penetration was significantly restrained.Due to the Si-F bond between SiC and PVDF-HFP,the structural stability has been obviously enhanced,which could suppress the growth of lithium(Li) dendrite.Furthermore,some 3D reticulated Si nanowires are found on the surface of Li anode,which also greatly inhibit Li dendrites and result in irregular flakes of Li metal.Especially,the shrinkage of 6% SiC/PVDF-HFP at 150℃ is only 5%,which is notably lower than those of PVDF-HFP and Celgard2500.The commercial LiFePO_(4) cell assembled with 6% SiC/PVDF-HFP possesses a specific capacity of 157.8 mA h g^(-1) and coulomb efficiency of 98% at 80℃.In addition,the tensile strength and modulus of 6% SiC/PVDF-HFP could reach 14.6 and 562 MPa,respectively.And a small deformation(1000 nm) and strong deformation recovery are obtained under a high additional load(2.3 mN).Compared with PVDF-HFP and Celgard2500,the symmetric Li cell assembled with 6% SiC/PVDF-HFP has not polarized after 900 cycles due to its excellent mechanical stabilities.This strategy provides a feasible solution for the composite separator of high-safety batteries with a high temperature and impact resistance.

关键词： SiC PVDF-HFP Composite separator Thermal stability Mechanical stability High safety battery

Mesoporous Silica （HMS） Based Composite Adsorbents and Its CO2 Adsorption Performance

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功能材料信息 2016年第3期13卷 48-48页

作者： Jie Liu Qian Tan Junsong Bai Jianying Liu Chenghua Xu Shengyu Liu Changwu Zou wanglai cen Chengdu University of Information Technology Chengdu 610225 P.R. China Air Environmental Modeling and Pollution Controlling Key Laboratory of Sichuan Higher Education Institutes Chengdu 610225 P.R. China Institute of New Energy and Low-Carbon Technology Sichuan University Chengdu 610065 P.R. China

K掺杂C_3N_4的原位合成、禁带结构解析及其可见光催化性能增强机制

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科学通报 2016年第24期61卷 2707-2716页

作者：李欣蔚张会均文莉董帆岑望来吴忠标重庆工商大学催化与功能有机分子重庆市重点实验室环境与资源学院重庆400067 四川大学新能源与低碳技术研究院成都610065 浙江大学环境工程系环境污染修复与生态健康教育部重点实验室杭州310027

以硫脲和碘化钾为原料,采用热聚合法合成了K掺杂g-C_3N_4光催化剂(CN-K),通过X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线能谱(XPS)、比表面积(BET)、紫外-可见漫反射(UV-vis DRS)和荧光光谱(PL)等对样品进行微... 详细信息

以硫脲和碘化钾为原料,采用热聚合法合成了K掺杂g-C_3N_4光催化剂(CN-K),通过X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线能谱(XPS)、比表面积(BET)、紫外-可见漫反射(UV-vis DRS)和荧光光谱(PL)等对样品进行微结构表征分析,并在优化晶体结构模型基础上,采用第一性原理计算模拟并解析能带结构和态密度分布.结果表明,掺杂K离子与N形成K–N键,并存在于g-C_3N_4层间.在可见光照射下对ppb级NO表现出了显著增强的可见光催化活性和良好的光化学稳定性.CN-K优异的活性可归因于K掺杂作用对g-C_3N_4电子结构的调变.K掺杂作用调节禁带位置,价带与导带的位置均下移,其中导带下移幅度高于价带,使催化剂禁带宽度减小,因此拓宽了光响应范围,使其可见光区域吸光能力增强;K掺杂使光生载流子的分离效率增加;K掺杂g-C_3N_4比纯g-C_3N_4的价带位置更正,K的掺杂作用使其光生空穴的氧化能力增强.本文阐明了K掺杂g-C_3N_4改性作用机理以及其可见光催化净化NO的机理.本文为光催化剂碱金属改性降解污染物提供了新的认识.

关键词： g-C3N4 K掺杂可见光催化禁带结构 NO净化

活性氧自由基生成及传输对g-C_3N_4上NO光催化去除的影响:原位红外光谱与计算模拟结合法（英文）

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Chinese Journal of Catalysis 2018年第10期39卷 1695-1703页

作者：李解元颜萍李康璐岑望来于晓巍袁山东楚英豪王正明四川大学建筑与环境学院四川大学新能源与低碳技术研究院环保部华南环境科学研究所日本产业技术综合研究所

石墨相氮化碳(g-C_3N_4)具有独特的二维层状结构和合适的能带结构,因而在可见光催化领域广受关注.尤其是在可见光去除环境污染物领域,得到了较为充分的研究与应用.然而g-C_3N_4去除环境污机理的反应机理尚不明确.因此,本文采用理论计算... 详细信息

石墨相氮化碳(g-C_3N_4)具有独特的二维层状结构和合适的能带结构,因而在可见光催化领域广受关注.尤其是在可见光去除环境污染物领域,得到了较为充分的研究与应用.然而g-C_3N_4去除环境污机理的反应机理尚不明确.因此,本文采用理论计算与实验高度结合的研究方法,以光催化NO去除为例,深入阐述了光照下g-C_3N_4表面活性氧物种(ROS)的生成及转化过程,及其介导下的NO光催化氧化机理.X射线衍射结果表明,g-C_3N_4是三嗪环层内聚合后层层堆叠而成,并由红外光谱确定了其表面的官能团类型.该结构经扫描电镜和透射电镜得到了进一步的验证.采用光致激发谱和紫外可见漫反射光谱等实验表征与密度泛函理论计算结合的光电性质分析,我们发现,g-C_3N_4在可见光下具有一定的响应,这为其在光催化去除NO中奠定了基础.同时,其价带位置过高,无法自行产生氧化性较强的羟基自由基(.OH).电子自旋共振技术结果表明g-C_3N_4在光照下能捕获到·O_2^-和·OH两种活性自由基.采用反应路径计算发现,·OH是由·O_2^-在导带上逐步得到电子被还原而生成,其中的速率控制步骤是H_2O_2的解离.因此,促进O_2分子的吸附和活化和克服H_2O_2解离的反应活化能是产生·OH和提升g-C_3N_4光催化氧化活性的关键.采用原位红外光谱技术对g-C_3N_4上NO的氧化去除过程进行了表征,发现其主要中间产物为NO_2,主要终产物为NO_2^-和NO_3^-,采用反应路径计算对该反应过程进行了理论模拟,发现在·O_2^-介导下,最高反应活化能为0.66 eV,而在·OH介导下,该活化能降低至0.46 eV,表明·OH的氧化性要明显强于·O_2^-.总之,本文采用一种可行的、高度结合的实验与计算手段研究了g-C_3N_4上ROS的生成及转化过程及其对NO去除的反应历程,在原子尺度揭示了该反应的机理,加深了对ROS在光催化环境污染物降解过程中作用的理解.

关键词：光催化活性氧物种石墨相氮化碳 NO去除反应机理