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Bending Resistance Covalent Organic Framework Superlattice:“Nano‑Hourglass”‑Induced Charge Accumulation for Flexible In‑Plane Micro‑Supercapacitors

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Nano-Micro Letters 2023年第2期15卷 198-211页

作者： Xiaoyang Xu Zhenni Zhang Rui Xiong Guandan Lu Jia Zhang Wang Ning shuozhen hu Qingliang Feng Shanlin Qiao College of Chemistry and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018People’s Republic of China State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237People’s Republic of China School of Chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi’an 710072People’s Republic of China Hebei Electronic Organic Chemicals Engineering Center Shijiazhuang 050018People’s Republic of China

Covalent organic framework(COF)film with highly exposed active sites is considered as the promising flexible selfsupported electrode for in-plane microsupercapacitor(MSC).Superlattice configuration assembled alternately by different nanofilms based on van der Waals force can integrate the advantages of each isolated layer to exhibit unexpected performances as MSC film electrodes,which may be a novel option to ensure energy output.Herein,a mesoporous free-standing A-COF nanofilm(pore size is 3.9 nm,averaged thickness is 4.1 nm)with imine bond linkage and a microporous B-COF nanofilm(pore size is 1.5 nm,averaged thickness is 9.3 nm)withβ-keto-enamine-linkages are prepared,and for the first time,we assembly the two lattice matching films into sandwich-type superlattices via layer-by-layer transfer,in which ABA–COF superlattice stacking into a“nano-hourglass”steric configuration that can accelerate the dynamic charge transportation/accumulation and promote the sufficient redox reactions to energy storage.The fabricated flexible MSC–ABA–COF exhibits the highest intrinsic CV of 927.9 F cm^(−3) at 10 mV s^(−1) than reported two-dimensional alloy,graphite-like carbon and undoped COF-based MSC devices so far,and shows a bending-resistant energy density of 63.2 mWh cm^(−3) even after high-angle and repeat arbitrary bending from 0 to 180°.This work provides a feasible way to meet the demand for future miniaturization and wearable electronics.

关键词： In-plane micro-supercapacitor Covalent organic framework Free-standing nanofilm Superlattice Bending resistance

Positive direction of polarization-induced electric field improves formic acid electrooxidation on Pd

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Nano Research 2023年第8期16卷 10848-10856页

作者： shuozhen hu Yunyun Cheng Guoming Luo Kai huang Cheng Shi Jie Xu Cheng Lian Shigang Sun Xinsheng Zhang State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Shanghai Hydrogen Propulsion Technology Co. Ltd.Shanghai 201800China Shanghai Haizhiqing Energy Development Co. Ltd.Shanghai 200333China Key Laboratory of Advanced Civil Engineering Materials of Ministry of Education Functional Materials Research LaboratorySchool of Materials Science and EngineeringTongji UniversityShanghai 201804China School of Materials Science and Engineering Anhui University of TechnologyMa’anshan 243002China State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Adjusting the adsorption energy of adsorbates on catalyst can directly regulate the catalytic performance and reaction pathways of heterogeneous catalysis.Herein,we report a novel strategy,introducing polarization-induced electric field(PIEF)with different directions,to manipulate the adsorption energy of intermediates and reaction pathway of formic acid electrooxidation on Pd.Tourmaline nanoparticles are applied as the PIEF provider,of which the direction is successfully controlled via aligning the dipoles in tourmaline in a strong external electric field.Experimental and theoretical results systematically reveal that positive PIEF leads to an electron-deficient state of Pd,reduced adsorption energy of COad,enhanced adsorption energy of*HCOOH and*OH,and promoted formate pathway of formic acid electrooxidation.Pd/TNP+/FTO,with the aid of positive PIEF,shows three-fold enhancement in the formic acid electrooxidation(4.74 mA·cm^(−2))with high durability and anti-poisoning ability compared with pristine Pd.This study leads a new route to design formic acid electrocatalysts and provides an understanding on how to control the adsorption energy of adsorbates on electrocatalysts by an internal electric field.

关键词： dipole-aligned tourmaline ferroelectric material polarization-induced electric field direction palladium adsorption energy formic acid oxidation mechanism

SDS-modified Nanoporous Silver as an Efficient Electrocatalyst for Selectively Converting CO2 to CO in Aqueous Solution

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Chinese Journal of Chemistry 2019年第4期37卷 337-341页

作者： Lei Shi Yuning Zhang Xiaofei Han Dongfang Niu Jinlong Sun Jenny Y.Yang shuozhen hu Xinsheng Zhang State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Department of Chemistry University of CaliforniaIrvineCalifornia 92697United States

Selectively electrochemical conversion of CO2 into organic fuel using renewable electricity is one of the most sought-after processes.In this paper,we report the electrochemical reduction of CO2(CO2RR)on the nanoporous Ag electrodes made of compacted Ag nanoparticles(AgNPs),which were prepared by one-step reduction in the water phase with or without the surfactant sodium dodecyl sulfate(SDS).The scanning electron microscope(SEM)characterizations show that the compacted Ag electrodes have the nanoporous morphology formed by stacking AgNPs.Compared with the nanoporous Ag electrode without SDS modification(C-AgNPs),the SDS-modified AgNPs electrode(C-AgNPs-SDS)is highly effective in improving selective CO production in a wide range of potentials(-0.69 V--1.19 V,vs.RHE),with a Faradaic efficiency of 92.2% and a current density of -8.23 mA·cm^-2 for CO production at -0.79 V(vs.RHE).C-AgNPs-SDS is also catalytically stable with only less than 7% deactivation after 8 h of continuous electrolysis.

关键词： CO2 CO Aqueous Solution

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电化学法处理香料工业氯化钠有机废盐的研究

无机盐工业 2024年第3期56卷 105-115页

作者：姚健康胡硕真钮东方吴建平张新胜华东理工大学化学工程联合国家重点实验室上海200237 上海瑞元化学科技有限公司上海200231

为了实现氯化钠有机废盐的资源化利用,以某香料企业的氯化钠有机废盐为研究对象,在单室电化学氧化的基础上提出了一种资源化处理氯化钠废盐的一膜两室电解工艺,在降解废盐有机物的同时获取氢氧化钠。在单室电解槽中探究了废盐中有机物... 详细信息

为了实现氯化钠有机废盐的资源化利用,以某香料企业的氯化钠有机废盐为研究对象,在单室电化学氧化的基础上提出了一种资源化处理氯化钠废盐的一膜两室电解工艺,在降解废盐有机物的同时获取氢氧化钠。在单室电解槽中探究了废盐中有机物的电化学氧化降解条件和降解途径,研究表明,在电流密度为600 A/m^(2)、反应温度为35℃、初始pH为6的最佳电解条件下,电解8 h后废盐模拟废水化学需氧量(COD)去除率为92.3%,色度去除率为100%,电流效率为32.3%。有机物降解的主要途径为电极产生的活性氯和羟基自由基对有机物的间接氧化。通过调节阳极液pH和进料方式,在相同电解条件下电解8 h,一膜两室工艺阳极COD去除率可达87.2%,阴极氢氧化钠总产量可达11.33 g。该工艺具有反应条件温和、工艺流程简单及无二次污染等特点,可为氯化钠有机废盐的资源化处理提供参考。

关键词：电化学氯化钠有机废盐有机物降解途径资源化

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二苯甲酮腙电氧化制备二苯重氮甲烷的研究

有机化学 2024年第3期44卷 951-965页

作者：韩璐瑶胡硕真郭庆春郭红永高照群许颖张新胜华东理工大学化工学院上海200237 河北兰升生物科技有限公司河北石家庄052260

研究了二苯甲酮腙电催化氧化合成二苯重氮甲烷.针对二苯重氮甲烷的不稳定特性,通过非均相电解体系设计,优选卤化合物、电解质种类、反应溶剂的极性以及电极材料、控制电流密度和反应温度等措施,抑制过氧化副产物二苯甲酮、水解副产物二... 详细信息

研究了二苯甲酮腙电催化氧化合成二苯重氮甲烷.针对二苯重氮甲烷的不稳定特性,通过非均相电解体系设计,优选卤化合物、电解质种类、反应溶剂的极性以及电极材料、控制电流密度和反应温度等措施,抑制过氧化副产物二苯甲酮、水解副产物二苯甲醇及偶联副产物二苯甲酮吖嗪的生成,以74%的高收率获得二苯重氮甲烷.此外,还初步探究了二苯甲酮腙电氧化机理.

关键词：间接电合成非均相电解二苯重氮甲烷碘化合物

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脉冲压缩在铝薄板电磁超声导波检测中的应用

航空学报 2022年第3期43卷 509-520页

作者：石文泽程进杰胡硕臻卢超陈尧南昌航空大学无损检测教育部重点实验室南昌330063 中国科学院声学研究所声场声信息国家重点实验室北京100190 赣南师范大学江西省数值模拟与仿真技术重点实验室赣州341000

针对电磁超声换能器(EMAT)换能效率低导致超声回波信噪比(SNR)差这一问题,基于相位编码脉冲压缩技术,讨论了匹配滤波器及旁瓣抑制滤波器的设计及其在电磁超声检测中的实现。选用典型二相编码信号-巴克码作为激励信号,分析了不同码长、... 详细信息

针对电磁超声换能器(EMAT)换能效率低导致超声回波信噪比(SNR)差这一问题,基于相位编码脉冲压缩技术,讨论了匹配滤波器及旁瓣抑制滤波器的设计及其在电磁超声检测中的实现。选用典型二相编码信号-巴克码作为激励信号,分析了不同码长、载波周期数的巴克码信号对电磁超声导波检测脉冲压缩效果的影响,并研究了旁瓣抑制算法的效果。以含人工预制裂纹的7075航空铝合金薄板为检测对象,选用SH;模态电磁超声导波换能器对比了单频正弦信号激励方式与巴克码脉冲压缩技术获得的缺陷回波信号信噪比。结果表明,采用巴克码脉冲压缩后超声回波的信噪比较单频正弦激励方式至少提高了7.2 dB,且巴克码脉冲压缩技术能探测出单频正弦激励方式而不能可靠检出的小裂纹(长×宽×深为10.0 mm×1.0 mm×0.25 mm)。将相位编码压缩技术应用于电磁超声导波检测,可达到增加EMAT提离和减小同步平均次数的目的,能满足在线快速检测的需求。

关键词：铝合金 EMAT SH 导波巴克码脉冲压缩

酞菁钴催化剂载体表面含氮官能团对其在燃料电池中氧还原性能的影响

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化学学报 2018年第9期76卷 723-728页

作者：黄文姣张浩宇胡硕真钮东方张新胜华东理工大学化学工程联合国家实验室上海200237

以酞菁钴为催化剂,纳米碳管为载体,分别通过超声法和四氢呋喃法混合分散,并在氮气氛围高温热处理制备了两种酞菁钴催化剂.热重分析(TGA)结果显示超声法制备的酞菁钴催化剂(CoPc-CNT-S)含钴的质量分数为8.1 wt%,四氢呋喃混合法制备的酞... 详细信息

以酞菁钴为催化剂,纳米碳管为载体,分别通过超声法和四氢呋喃法混合分散,并在氮气氛围高温热处理制备了两种酞菁钴催化剂.热重分析(TGA)结果显示超声法制备的酞菁钴催化剂(CoPc-CNT-S)含钴的质量分数为8.1 wt%,四氢呋喃混合法制备的酞菁钴催化剂(CoPc-CNT-R)含钴的质量分数为7.0 wt%.X射线光电子谱(XPS)结果显示CoPc-CNT-R催化剂的含氮量是CoPc-CNT-S催化剂的两倍多,且两种催化剂含氮官能团的种类及比例不同.相比较而言,CoPc-CNT-S表面有更多的吡咯型氮.将两种催化剂应用于混合酸碱燃料电池中发现:CoPc-CNT-S对电催化氧还原有较高的活性和稳定性,将CoPc-CNT-S作为燃料电池的阴极催化剂分别工作5 h和15 h后,电荷转移电阻相对CoPc-CNT-R为阴极催化剂时均较低.原因可能是相近比例的吡啶型N和吡咯型N的协同作用有利于电催化氧还原.

关键词：非贵金属催化剂酞菁钴纳米碳管燃料电池电催化氧还原