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Nano Research 2024年第6期17卷 4882-4888页

作者： Shuai Qi Jinlian Liao Kunzhong Chen Senkai Li Jinwen Zhao Tianchi Huang Na Meng hengpan yang Qi Hu Chuanxin He College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China

Developing non-precious metal-based bifunctional electrocatalysts capable for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to achieve efficient water electrolysis for mass hydrogen production,however it remains challenging.Here,we report the synthesis of hierarchical nanorod arrays comprising core-shell structured P-doped NiMoO4@NiFe-coordination polymer(denoted as P-NiMoO4@NiFeCP)as bifunctional electrocatalysts for water electrolysis.Furthermore,we systematically investigate the influence of NiFeCP shell thickness on electrocatalytic activity,manifesting the presence of strong interfacial synergetic effect between P-NiMoO4 and NiFeCP for boosting both the HER and OER.With advantageous hierarchical architectures and unique core-shell structures,optimized P-NiMoO_(4)@NiFeCP-7.3(7.3 is the shell thickness in nm)requires overpotentials of merely 256 and 297 mV to yield a current density of 1000 mA·cm^(−2)for the HER and OER in 1 M KOH,respectively.More importantly,it can serve as a bifunctional electrocatalyst for efficient and sustainable overall water electrolysis,delivering large current densities of 500 and 1000 mA·cm^(−2)at low cell voltages of 1.804 and 1.865 V,along with high stability of over 500 h at 1000 mA·cm−2,demonstrating the great potential of this electrocatalyst towards practical applications.

关键词： hydrogen evolution reaction oxygen evolution reaction overall water splitting non-precious metal-based electrocatalysts core-shell structures

Bimetallic two-dimensional materials for electrocatalytic oxygen evolution

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Chinese Chemical Letters 2022年第8期33卷 3657-3671页

作者： Xiaojie Li Qi Hu hengpan yang Tao Ma Xiaoyan Chai Chuanxin He College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China

Electrocatalytic oxygen evolution reaction(OER)is one of the important half reactions of electrocatalytic water splitting.However,the slow kinetic process involving four-electron transfer severely limits its reaction efficiency,which in turn limits the overall electrocatalytic hydrolysis efficiency.In order to improve the activity of the electrocatalytic OER,researchers mainly update the catalyst from three aspects,that is,increase the conductivity of the electrocatalyst,and the quantity and quality of active sites.Twodimensional(2 D)engineering can effectively reduce the resistance of the materials and greatly increase the number of electrochemically active sites,while heterometal doping,or the bimetal strategy,can improve the quality of active sites via changing the electronic structure of the material.Thus,the combination of the two can enhance the activity of electrocatalytic OER in all three aspects:conductivity,number and quality of active sites.However,there is currently no review on this topic.Therefore,in this review,we summarize the application of bimetallic 2 D materials in electrocatalytic OER from four aspects:the structure,synthesis strategy,catalytic efficiency,and reaction mechanism.

关键词： Bimetal/bimetallic Two-dimensional/2D Oxygen evolution Electrocatalytic MOF LDH

A hierarchically structured tin-cobalt composite with an enhanced electronic effect for high-performance CO_(2) electroreduction in a wide potential range

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Journal of Energy Chemistry 2023年第1期76卷 462-469,I0012页

作者： Xingxing Jiang Xuan Li Yan Kong Chen Deng Xiaojie Li Qi Hu hengpan yang Chuanxin He Institute of Microscale Optoelectronics College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060GuangdongChina

Earth-abundant and nontoxic Sn-based materials have been regarded as promising catalysts for the electrochemical conversion of CO_(2)to C1 products,e.g.,CO and formate.However,it is still difficult for Snbased materials to obtain satisfactory performance at low-to-moderate overpotentials.Herein,a simple and facile electrospinning technique is utilized to prepare a composite of a bimetallic Sn-Co oxide/carbon matrix with a hollow nanotube structure(Sn Co-HNT).Sn Co-HNT can maintain>90%faradaic efficiencies for C1 products within a wide potential range from-0.6 VRHE to-1.2 VRHE,and a highest 94.1%selectivity towards CO in an H-type cell.Moreover,a 91.2%faradaic efficiency with a 241.3 m A cm^(-2)partial current density for C1 products could be achieved using a flow cell.According to theoretical calculations,the fusing of Sn/Co oxides on the carbon matrix accelerates electron transfer at the atomic level,causing electron deficiency of Sn centers and reversible variation between Co^(2+)and Co^(3+)centers.The synergistic effect of the Sn/Co composition improves the electron affinity of the catalyst surface,which is conducive to the adsorption and stabilization of key intermediates and eventually increases the catalytic activity in CO_(2)electroreduction.This study could provide a new strategy for the construction of oxide-derived catalysts for CO_(2)electroreduction.

关键词： Hierarchic structure Tin-cobalt bimetallic oxide Electronic effect CO_(2)electroreduction Wide potential range

Janus heterostructure of cobalt and iron oxide as dual-functional electrocatalysts for overall water splitting

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Nano Research 2023年第2期16卷 2245-2251页

作者： Xiaojie Li Huike Zhang Xuan Li Qi Hu Chen Deng Xingxing Jiang hengpan yang Chuanxin He College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China Institute of Microscale Optoelectronics Shenzhen UniversityShenzhen 518060China

In electrocatalytic water splitting,low-cost dual-functional catalysts can not only reduce costs but also avoid cross-contamination of cathode and anode.However,the orderly aggregation of active sites for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)into a specific catalyst is very challenging.In this study,a Co/Fe_(3)O_(4)Janus heterojunction supported on carbon fiber paper(J-CoFe-CFP)is designed and successfully synthesized.Generally,Co-Fe oxides have preferable OER activity but weak HER activity.However,in J-CoFe-CFP,due to the intense and special electronic interaction of different substances(Co and Fe3O4)in the Janus heterogeneous interface,a huge number of tidy high-quality HER and OER active sites are uniformly distributed on the interface simultaneously,which endows the catalyst with both excellent HER and OER performance.In HER,the overpotential@10 mA·cm^(−2)(ηHER)is only 53.9 mV,and the Tafel slope is 43.7 mV·dec^(−1).In OER,theηis 272 mV,and the Tafel slope is 50.2 mV·dec^(−1),much lower than those of RuO_(2)/CFP.In the J-CoFe-CFP||J-CoFe-CFP two-electrode system,the required voltage is only 1.26 V at the beginning and 1.56 V@10 mA·cm^(−2),much lower than those of RuO_(2)/CFP||20%Pt/C/CFP.This work provides a Janus heterojunction pathway for bifunctional water electrolysis catalysts.

关键词： Janus bifunctional electrocatalytic water splitting CoFe

Fluorine-induced dual defects in NiP_(2) anode with robust sodium storage performance

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Nano Research 2022年第3期15卷 2147-2156页

作者： Liang Wu Lifeng Wang Xiaolong Cheng Mingze Ma Ying Wu Xiaojun Wu hengpan yang Yan Yu Chuanxin He College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen 518060China Hefei National Laboratory for Physical Sciences at the Microscale Department of Materials Science and EngineeringCAS Key Laboratory of Materials for Energy ConversionUniversity of Science and Technology of ChinaHefei 230026China

Metal phosphides have shown great application potential as anode for sodium-ion batteries(NIBs)owing to high theoretical capacity,suitable operation voltage and abundant resource.Unfortunately,the application of NiP_(2) anode is severely impeded by low practical capacity and fast capacity decay due to the huge volume variation and low reactivity of internal phosphorus(P)component towards Na^(+).Herein,electronic structure modulation of NiP_(2) via heteroatoms doping and introducing vacancies defects to enhance Na+adsorption sites and diffusion kinetics is successfully attempted.The as-synthesized three-dimensional(3D)bicontinuous carbon matrix decorated with well-dispersed fluorine(F)-doped NiP_(2) nanoparticles(F-NiP_(2)@carbon nanosheets)delivers a high reversible capacity(585 mAh·g^(−1) at 0.1 A·g^(−1))and excellent long cycling stability(244 mAh·g^(−1) over 1,000 cycles at 2 A·g^(−1))when tested as anode in NIBs.Density functional theory(DFT)calculations reveal that F doping in NiP_(2) induces the formation of P vacancies with increased Na+adsorption energy and accelerates the alloying of internal P component.The F-NiP_(2)@carbon nanosheets//Na_(3)V_(2)(PO_(4))_(3) full cell is evaluated showing stable long cycling life.The heteroatoms doping-induced dual defects strategy opens up a new way of metal phosphides for sodium storage.

关键词： NiP_(2) electronic structure modulation F doping P vacancies dual defects sodium-ion batteries

Grain Boundaries Engineering of Hollow Copper Nanoparticles Enables Highly Efficient Ammonia Electrosynthesis from Nitrate

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CCS Chemistry 2022年第6期4卷 2053-2064页

作者： Qi Hu Yongjie Qin Xiaodeng Wang Hongju Zheng Keru Gao hengpan yang Peixin Zhang Minhua Shao Chuanxin He College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdong 518060 Department of Chemical and Biological Engineering and Energy Institute The Hong Kong University of Science and TechnologyKowloonHong Kong 999077

Electrochemical nitrate reduction reaction(NO_(3)−RR)is an ideal route to produce ammonia(NH_(3))under ambient conditions.Although a markedly improved NH3 production rate has been achieved on the NO_(3)−RR compared with the nitrogen reduction reaction(NRR),the NH_(3) production rate of NO_(3)−RR is still well below the industrial Haber-Bosch route due to the lack of robust electrocatalysts for yielding high current densitieswith concurrently good suppression of hydrogen evolution reaction(HER).Herein,we describe an in situ electrochemical strategy for the synthesis of hollow carbon-coated Cu nanoparticles(NPs)(HSCu@C)with abundant grain boundaries(HSCu-AGB@C)for highly efficient NO_(3)−RR in both alkaline and neutral media.Impressively,in alkaline media,the HSCu-AGB@C can achieve a maximum NH3 Faradaic efficiency of 94.2% with an ultrahigh NH_(3) rate of 487.8 mmol g^(−1) cat h^(−1) at−0.2 V versus a reversible hydrogen electrode,more than 2.4-fold of the rate obtained in the Haber-Bosch.Both theoretic computations and experimental results uncover that the grain boundaries play the key to improve the NO_(3)−RR performance.Herein,the industrial-scale NH_(3) production ratemay open exciting opportunities for the practical electrosynthesis NH_(3) under ambient conditions.

关键词： grain boundaries hollow structures artificial ammonia production nitrate reduction reaction Haber-Bosch route

Construction of cobalt-copper bimetallic oxide heterogeneous nanotubes for high-efficient and low-overpotential electrochemical CO_(2) reduction

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Journal of Energy Chemistry 2021年第3期30卷 1-6页

作者： Zhong Cheng Xiaodeng Wang hengpan yang Xinyao Yu Qing Lin Qi Hu Chuanxin He College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongChina

Currently,global warming and energy problems become more and more serious with the development of economy and the continuous consumption of fossil fuel,which are due to the release of greenhouse gas in the process of ... 详细信息

关键词： CO_(2)reduction reaction Electrocatalysts Bimetal Nanotube Selectivity

充分稳定和暴露的铜基异质结实现CO_(2)高效电还原制乙醇

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Chinese Journal of Catalysis 2024年第3期58卷 216-225页

作者：蒋兴星赵雨昕孔艳孙建桔冯上照胡琪杨恒攀何传新深圳大学化学与环境工程学院广东深圳518060

二氧化碳(CO_(2))虽然被视为破坏生态环境的温室气体,但也是储量最丰富的碳资源,对其进行转化和利用将对社会环境和能源结构产生深远影响.电化学还原CO_(2)(CO_(2)RR)不仅转化效率高,而且成本较低,有望实现规模化生产.在众多催化剂中,... 详细信息

二氧化碳(CO_(2))虽然被视为破坏生态环境的温室气体,但也是储量最丰富的碳资源,对其进行转化和利用将对社会环境和能源结构产生深远影响.电化学还原CO_(2)(CO_(2)RR)不仅转化效率高,而且成本较低,有望实现规模化生产.在众多催化剂中,廉价易得的铜基催化剂被认为是电化学催化还原CO_(2)生成高附加值产物的理想催化剂之一,其中铜氧化物的存在是CO_(2)RR生成高附加值产物的关键.然而,CO_(2)RR过程是在负电位下进行的,当施加电位低于‒0.1 VRHE时,铜氧化物很容易被还原为金属态铜.因此,催化剂稳定氧化态铜的能力在保持连续、高效和稳定的CO_(2)RR产多碳产物性能中至关重要.本文将简单的O_(2)等离子体处理技术与静电纺丝技术相结合,合成了多孔碳纳米纤维负载的Cu/Cu_(x)O异质结催化剂,并考察了其催化CO_(2)RR的性能.在静电纺丝过程中,Cu-ZIF-8前驱体的加入使得热处理后的原丝纤维中形成了丰富的网络贯穿多孔结构,该结构有效地实现了铜纳米颗粒的均匀分散;随后,通过O_(2)等离子体处理技术,在碳纳米纤维中构建了大量的开放介孔,为CO_(2)的吸附和反应提供了有利环境,并使Cu/Cu_(x)O异质结位点暴露于反应界面.电化学性能测试结果表明,在400 mA cm^(‒2)电流密度下,独特的Cu/Cu_(x)O异质结活性位点电催化还原CO_(2)生成乙醇的法拉第效率可达70.7%,该性能优于未经O_(2)等离子体处理的多孔铜纳米纤维.此外,高暴露的Cu/Cu_(x)O异质结活性位点显著地增加实际参与反应的活性位点数量,经计算Cu/Cu_(x)O异质结CO_(2)RR产乙醇的质量活性高达8.4 A mg^(‒1),是目前报道生产乙醇的较高质量活性.多孔碳纳米纤维衬底不仅具有协同电子输运能力,而且在CO_(2)RR测试中施加的负电压有助于维持Cu/Cu_(x)O异质结构的稳定性,使其在高电流密度下能够保持长时间的催化稳定性.此外,本文利用原位拉曼光谱和红外光谱、有限元模拟及密度泛函理论计算等方法深入研究了Cu/Cu_(x)O异质结的催化机理.原位拉曼光谱和红外光谱表征结果证实了在CO_(2)RR过程中Cu_(x)O的动态稳定状态以及关键信号*CO和C‒C键的存在;理论计算表明,Cu/Cu_(x)O异质结的存在促进了关键中间体*CO的溢流,降低了C‒C耦合过程的反应能垒,从而提高了还原产物乙醇的产率.综上,本文成功地在多孔铜纳米纤维中引入氧化物物种,并优化了纤维孔结构.其表现出了较好的电催化还原CO_(2)性能,可高选择性生成乙醇,其独特的多孔碳纤维结构充分暴露了活性位点,实现了较高的质量活性.本文所采用的催化剂组分和微观结构的调控策略为提升电催化中催化剂稳定性和催化活性提供了有益的借鉴.

关键词：二氧化碳电还原 Cu/Cu_(x)O异质结开口孔结构质量活性乙醇

钴单原子的双重限域制备策略及高效CO_(2)电还原性能

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高等学校化学学报 2022年第9期43卷 156-165页

作者：吴玉李轩杨恒攀何传新中国科学技术大学化学物理系合肥微尺度物质科学国家实验室合肥230026 深圳大学化学与环境工程学院深圳功能高分子重点实验室深圳518071

将锌钴双掺杂的金属有机框架(MOFs)纳米颗粒(ZnCo-ZIF)与聚丙烯腈(PAN)混溶形成前驱体溶液,通过静电纺丝与高温热化学反应,获得了一种多孔碳纳米纤维负载的钴单原子催化剂(A-Co@PCFs).高温热解时,聚丙烯腈分解碳化形成碳纳米纤维主体,M... 详细信息

将锌钴双掺杂的金属有机框架(MOFs)纳米颗粒(ZnCo-ZIF)与聚丙烯腈(PAN)混溶形成前驱体溶液,通过静电纺丝与高温热化学反应,获得了一种多孔碳纳米纤维负载的钴单原子催化剂(A-Co@PCFs).高温热解时,聚丙烯腈分解碳化形成碳纳米纤维主体,MOFs纳米颗粒结构坍塌伴随锌组分的挥发,在纤维表面形成了丰富的多级孔结构.由于碳纳米纤维和孔道结构的双重限域作用,使钴组分不能聚集成钴纳米颗粒,而是形成高度分散的钴单原子.电化学测试结果表明,该钴单原子催化剂可将CO_(2)电还原为CO,在−0.66 V(vs.RHE)下,CO的法拉第效率可达94%.并且经过60 h的耐久性测试,其催化性能没有明显的性能衰减,显示出较高的稳定性.A-Co@PCFs的高活性与高稳定性可归因于材料的多孔结构和高度分散的钴原子,这也使其具有代替贵金属催化剂的可能性.

关键词：静电纺丝碳纳米纤维双重限域单原子二氧化碳还原

A time-released osmotic pump fabricated by compression-coated method: Formulation screen, mechanism research and pharmacokinetic study

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Asian Journal of Pharmaceutical Sciences 2014年第4期9卷 208-217页

作者： Tiegang Xin yang Zhao hengpan Jing Wenji Zhang Yunyun Gao Xinggang yang Xukai Qu Weisan Pan Department of Pharmaceutics School of PharmacyShenyang Pharmaceutical University103 Wenhua RoadShenyang 110016China College of Pharmaceutical Science Zhejiang University of Technology18 Chaowang RoadHangzhou 310014China State Key Laboratory of Drug Delivery Technology and Pharmacokinetics Tianjin Institute of Pharmaceutical ResearchTianjin 300193China

In this investigation,time-released monolithic osmotic pump(TMOP)tablets containing diltiazem hydrochloride(DIL)were prepared on the basis of osmotic pumping mechanism.The developed dosage forms were coated by Kollidon®SR-Polyethylene Glycol(PEG)mixtures via compression-coated technology instead of spray-coating method to form the outer membrane.For more efficient formulation screening,a three-factor five-level central composite design(CCD)was introduced to explore the optimal TMOP formulation during the experiments.The in vitro tests showed that the optimized formulation of DIL-loaded TMOP had a lag time of 4 h and a following 20-h drug release at an approximate zero-order rate.Moreover,the releasemechanismwas proven based on osmotic pressure and its profile could be well simulated by a dynamic equation.After oral administration by beagle dogs,the comparison of parameters with the TMOP tablets and reference preparations show no significant differences for C_(max)(111.56±20.42,128.38±29.46 ng/ml)and AUC_(0-48 h)(1654.97±283.77,1625.10±313.58 ng h/ml)but show significant differences for T_(max)(13.00±1.16,4.00±0.82 h).These pharmacokinetic parameters were consistent with the dissolution tests that the TMOP tablets had turned out to prolong the lag time of DIL release.

关键词： Time-released Osmotic pump Compression-coated Central composite design Pharmacokinetic