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Journal of Energy Chemistry 2019年第1期28卷 73-78页

作者： Lijie Hou Jianing Guo zhonghua xiang State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology

For the sake of accelerating the commercial application of fuel cells, non-noble metal catalysts with high activity and high stability have been widely developed to replace platinum-based catalysts. Here, we report a simple but cost-effective synthetic strategy using iron tetra-amino phthalocyanine(FePC-NH_2)and modified carbon black(HCB) to obtain a novel oxygen reduction electrocatalyst(named as FePCNH_2/HCB-800) with Fe_2O_3 wrapped in nitrogen-doped carbon(N-carbon) as active site. The HCB as template can effectively promotes the formation of Fe_2O_3 active site in the catalysts. Compared to commercial Pt/C catalyst, the Fe PC-NH_2/HCB-800 catalyst exhibits high electrocatalytic activity for oxygen reduction reaction(ORR) with onset potential of 0.98 V and half-wave potential with 0.84 V vs. reversible hydrogen electrode(RHE). Meanwhile, the catalyst also shows excellent circulation stability. We believe that this work provides a platform for ORR and is conducive to the commercialization of fuel cells and metal-air batteries.

关键词： Oxygen reduction reaction Iron tetra-amino phthalocyanine Fuel cell Electrocatalyst

Advanced MOF-based electrode materials for supercapacitors and electrocatalytic oxygen reduction

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Nano Research 2023年第1期16卷 1338-1361页

作者： Bolong Yang Bingjie Li zhonghua xiang State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China The First Affiliated Hospital of Zhengzhou University Zhengzhou 450052China

Metal-organic frameworks(MOFs)have attracted a lot of attention due to their diverse structures,favorable porous properties,and tunable chemical compositions in the multiple ***,MOF-based materials(including pristine MOFs,MOF composites,and their derivatives)play the vital role in electrochemical energy storage and conversion systems,due to their ability for regulating chemical composition at the molecular level and their highly porous frameworks for facilitating the mass and charge *** and fuel cells are used as one of energy storage and conversion systems respectively,and it is unstoppable to design and synthesize high-efficiency electrode materials for *** review starts with the strategies for designing targeted MOF-based materials in electrochemical energy storage and conversion applications followed by the state-ofthe-art MOF-based materials discussed as to their potential applications in supercapacitors and electrocatalytic oxygen reduction reaction(ORR).Finally,the challenges and perspectives of MOF-based materials applied for supercapacitors and electrocatalytic ORR are discussed.

关键词： metal-organic frameworks(MOFs) MOF composites MOF derivatives supercapacitors electrocatalytic oxygen reduction reaction(ORR)

Three-dimensional nitrogen and phosphorous Co-doped graphene aerogel electrocatalysts for efficient oxygen reduction reaction

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Science China Chemistry 2018年第5期61卷 592-597页

作者： Jizhen Ma zhonghua xiang Jintao Zhang Key Laboratory for Colloid and Interface Chemistry Ministry of Education School of Chemistry and Chemical EngineeringShandong University State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology

The development of efficient electrocatalysts for oxygen reduction reaction(ORR) is of importance for fuel cells and metal-air batteries. Herein, three-dimensional nitrogen and phosphorous co-doped graphene aerogel(NPGA) was prepared via the pyrolysis of polyaniline(PANi) coated graphene oxide aerogel synthesized by oxidative polymerization of aniline on graphene oxide(GO) sheets in the presence of phytic acid. The uniform coating of PANi thin layer on the surface of GO sheets enables the formation of highly porous composite aerogel of PANi and GO. The subsequent thermal treatment is able to prepare the porous NPGA due to the carbonization of PANi and phytic acid as nitrogen and phosphorous resources. When used as electrocatalysts,the as-prepared NPGA electrocatalysts exhibited good catalytic activity to ORR via an efficient four-electron pathway with good stability, benefiting from the highly porous structure and the heteroatom co-doping. More importantly, Zn-air batteries operated in ambient air have been fabricated by coupling a Zn plate with the NPGA electrocatalyst in an air electrode, demonstrating the maximal power density as high as ~260 W/g and a good long-term stability with slightly potential decay for over 450 h. The facile method for preparing efficient carbon based ORR electrocatalysts would generate other potential applications including fuel cells and others.

关键词： graphene aerogel heteroatom doping oxygen reduction reaction Zn-air battery

N-rich covalent organic polymer in situ modified TiO_2 for highly efficient photocatalytic hydrogen evolution

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Science Bulletin 2018年第6期63卷 369-375页

作者： Zhuohang Zhou Peng Peng zhonghua xiang State Key Laboratory of Organic-Inorganic Composites College of Chemical Engineering College of Energy Beijing University of Chemical Technology

TiO2 has been everlastingly employed as popular photocatalyst for water splitting. However, the wide band gap （3.0-3.2 eV） and poor absorption to visible light of TiO2 result in a low utilization of solar energy and limit its large-scale application. To decrease its band gap and promote the utilization of full solar energy, we here modified TiO2 by in situ growth of N-rich covalent organic polymer （termed as COPuM）. During the in situ growth of COPuM on the surface of TiO2, intimate contacts between TiO2 and COPuM were built and core-shell structures were finally formed. The derived TiO2@COPHM demon-strated a narrower band gap （2.53 eV） compared to raw TiO2 （3.13 eV） and improved absorption to visible light. The optimal TiO2@COPHM hybrid exhibited excellent hydrogen evolution performance of 162.7μmol h^-1 under simulated sunlight which was more than 3 times higher than raw TiO2 （51.3μmol h^-1）. Particularly, visible light hydrogen evolution rate of TiO2@COPHM reached 0.65 μmol h^-1 while non-hydrogen generation was observed using raw TiO2.

关键词： Carbon nitrideCovalent organic polymers Water splitting Hydrogen generation Photocatalysis

Fluorinated bimetallic nanoparticles decorated carbon nanofibers as highly active and durable oxygen electrocatalyst for fuel cells

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Journal of Energy Chemistry 2022年第10期31卷 549-555,I0014页

作者： Yiming Leng Bolong Yang Yun Zhao zhonghua xiang State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China

The low activity and durability are still the critical barriers for non-precious metal electrocatalyst,mainly involving M-N/C(M=Fe,Co,Mn et al),applied in fuel *** bimetallic sites has been explored as an effective method to boost the performance of the catalyst for the synergistic effect between metal ***,this synergistic effect is always suppressed in acidic conditions and results in unstable catalytic *** we create novel fluorinated iron(Fe)and cobalt(Co)bimetallic nanoparticles distributed on nitrogen-doped carbon nanofibers(CNFs)for oxygen reduction reaction(ORR).The fluorination strongly increased the charge density of the bimetallic catalyst and resulted in a remarkable catalytic performance with the half-wave potential of 804 m V in 0.1 M HCl O_(4)and 1.6 times power density improvement for the proton exchange membrane fuel cell ***,the chemical and mechanical robust CNFs support improved the electric conductivity and stability of bimetallic catalysts,which leads to an ultra-stable *** fuel cell voltage can keep stable even after 110 h,instead of the continuingly decrease in the traditional M-N/C.

关键词： Bimetallic catalyst Fluorination Electrospinning ORR catalyst PEM fuel cell

Binary ligand strategy toward interweaved encapsulation-nanotubes structured electrocatalyst for proton exchange membrane fuel cell

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Journal of Energy Chemistry 2022年第1期31卷 129-135,I0005页

作者： Qingbin Liu Li Xu Shizhen Liu zhonghua xiang State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Petrochemical Research Institute PetroChina Company LimitedBlock 42.CNPC Innovation BaseChangping District.Beijing 102206.China

Hierarchically porous architecture of ir on-nitroge n-carb on(Fe-N-C)for oxyge n reducti on reaction(ORR)is highly desired towards efficient mass transfer in the fuel cell device ***,we reported a binary ligand strategy to prepare zeolitic imidazolate frameworks(ZIFs)-derived precursors,wherein the addition of secondary ligand endows precursors with the capabilities to transform into porously interweaved encapsulation-nanotubes structured composites after *** optimal catalyst,i.e.,termed as Fe_(6)-M/C-3,exhibits excellent durability with 88.8%current retention after 50,000 seconds in 0.1 M HClO_(4)solution by virtue of nanoparticles-encapsulation features,which is more positive than the benchmark commercial 20 wt%Pt/C ***,a promising maximum power density of Fe_(6)-M/C-3 as cathode catalyst was also dem on strated in proton exchange membrane fuel cells(PEMFCs)***,this binary ligand approach to the fabrication of hierarchically porous structures would also have significant implications for various other electrochemical reactions.

关键词： Oxygen reduction reaction Binary ligand strategy Interweaved encapsulation-nanotubes architecture Proton exchange membrane fuel cells

Secondary reduction strategy synthesis of Pt-Co nanoparticle catalysts towards boosting the activity of proton exchange membrane fuel cells

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Particuology 2023年第8期79卷 18-26页

作者： Bolong Yang Xiaogang Yu Jingkui Hou zhonghua xiang State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing100029China

Based on the volcanic relationship between catalytic activity and key adsorption energies,Pt-Co alloy materials have been widely studied as cathode oxygen reduction reaction(ORR)catalysts in proton exchange membrane fuel cells(PEMFCs)due to their higher active surface area and adjustable D-band energy levels compared to Pt/***,how to balance the alloying degree and ORR performance of Pt-Co catalyst remains a great ***,we first synthesized a well-dispersed Pt/Co/C precursor by using a mild dimethylamine borane(DMAB)as the reducing *** precursor was calcined at high temperature under H_(2)/Ar mixed gas by a secondary reduction strategy to obtain an ordered Pt_(3)Co intermetallic compound nanoparticle catalyst with a high degree of *** optimization of elec-tronic structure due to Pt-Co alloying and the strong metal-carrier interaction ensure the high kinetic activity of the cell membrane ***,the high degree of graphitization increases the electrical conductivity during the *** a result,the activity and stability of the catalyst were significantly improved,with a half-wave potential as high as 0.87 V,which decreased by only 20 mV after 10000 potential ***-cell tests further validate the high intrinsic activity of the ordered Pt_(3)Co catalyst with mass activity up to 0.67 A mg_(pt)^(-1),exceeding the United States Department of Energy(US DOE)standard(0.44 A mg_(pt)^(-1)),and a rated power of 5.93 W mg_(pt)^(-1).

关键词： Ordered Pt3Co nanoparticle Low platinum catalyst Secondary reduction strategy Oxygen reduction reaction Proton exchange membrane fuel cells

d-Orbital steered FeN_(4)moiety through N,S dual-site adjustation for zinc-air flow battery

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Journal of Energy Chemistry 2024年第5期92卷 8-15页

作者： Chunzhu Bao Mingwei Tong Xueli Li zhonghua xiang State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China

The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in synergistically regulating their electronic states and structural porosity for the great device ***,we conquer these issues by exploiting N and S co-doped graphene with COP rich in metal-ligand nitrogen to synergistically construct an effective catalyst for oxygen reduction reaction(ORR).Among them,the N and S co-doped sites with high electronegativity properties alter the number of electron occupations in the d orbital of the iron centre and form electron-transfer bridges,thereby boosting the selectivity of the ORR-catalysed four-electron ***,the introduction of COP materials aids the formation of pore interstices in the graphene lamellae,which both adequately expose the active sites and facilitate the transport of reactive *** from the synergistic effect,as-prepared catalyst exhibits excellent half-wave potentials(E_(1/2)=912 mV)and stability(merely 8.8%drop after a long-term durability test of 50000 s).Further,ZAFBs assembled with the N/SG@CO_(2)P catalyst demonstrate exceptional power density(163.8 mW cm^(-2))and continuous charge and discharge for approximately 140 h at 10 mA cm^(-2),outperforming the noble-metal benchmarks.

关键词： Nitrogen/sulfurdual sites Metal-coordinated nitrogen sites Covalent organic polymer Oxygen reduction reaction Zn-airflow battery

High retention volume covalent organic polymer for xenon capture:Dynamic separation of Xe and Kr

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Green Energy & Environment 2022年第5期7卷 948-956页

作者： Qian Wang Zhu Meng Juntao Li Shuming Peng zhonghua xiang Institute of Nuclear Physics and Chemistry China Academy of Engineering PhysicsMianyangSichuan621900China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing100029China Department of Chemistry Imperial College London20 Gordon StreetLondonWC1H0AJUK Department of Chemistry University College LondonLondonW120BZUK

Xenon capture and Xe/Kr separation are important processes in *** instance,Xe/Kr separation is an indispensable step in recycle and treatment of nuclear fuel *** different separation methods,selectively adsorb gas molecules using porous materials is a promising way to reduce the high energy consumption in traditional cryogenic ***,many reported adsorbents still face the challenges of:ⅰ) poor separation property at low Xe/Kr concentrations;ⅱ) insufficient retention volumes,which influence the viability of whole *** this work,we present a stable covalent organic polymer,i.e.,COP-14,showing promising potential for Xe/Kr *** dynamic breakthrough experiments,COP-14 successfully separates low concentration Xe(350 ppm) and Kr(35 ppm) from target gas ***,the xenon retention volume per gram(1700 mL g^(-1) at 298 K) of COP-14 in dynamics absorption process achieves 3.8 times of benchmark active *** good performance of the newly devloped COP-14 mainly from its rich nitrogen sites and suitable pore size with xenon *** promising results of COP-14 on Xe/Kr separation in this work provide a promising way for designing efficient Xe/Kr separation mateirals.

关键词： process separation retention

Microfluidic interface boosted synthesis of covalent organic polymer capsule

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Green Chemical Engineering 2020年第1期1卷 63-69页

作者： Yun Zhao Min Zhang Xin Wen zhonghua xiang State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing100029PR China

Microcapsules have been widely used in drug carriers,nano/microreactors,artificial organelles for their empty space and functional *** synthesized from spherical liquid-liquid interface show ultrathin shell and large ***,spherical liquid-liquid interfaces generated by stirring or sonicating are difficult in controlling the droplet size and preventing their coalescence,which results in inhomogeneous ***,we demonstrate a microfluidic interfacial synthetic method to produce microcapsules using the hot covalent organic polymers(COPs)coupled with Schiff-base reaction.A very high throughput of uniform and individual microdroplets about~1400 min^(-1)was generated under high flow rate for COP capsules *** catalyst promoted amine and aldehyde condensation that reacted less than 1 s assured the polymerization occurred at the liquid-liquid interface regardless of the diffusion intensification in microfluidic *** capsules with shell thickness around 50 nm were flexible enough to response to slight interior capillary force and exterior filtration force to form origami structure and sealed flat membrane,*** of the interfacial synthesized capsule expressed large capacity by encapsulating 1.41×10^(-2)μg SiO_(2)nanoparticles as theoretically ***,these properties make the COP capsules promising in,but not limited to,fast drug delivery and microreactors.

关键词： Covalent organic polymers Microcapsules Interfacial synthesis Microfluidic system High throughput