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One-pot synthesis of N-doped petroleum coke-based microporous carbon for high-performance CO_(2) adsorption and supercapacitors

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Journal of Environmental Sciences 2024年第5期139卷 93-104页

作者： Wenfu Zhu Yuqin Wang Fan Yao Xiaohong Wang Haoming Zheng Guangzheng Ye Hairong Cheng Junliang Wu Haomin Huang Daiqi Ye School of Environment and Energy South China University of TechnologyGuangzhou 510006China National Engineering Laboratory for VOCs Pollution Control Technology and Equipment Guangzhou 510006China Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control(SCUT) Guangzhou 510006China Guangdong Provincial Engineering and Technology Research Centre for Environmental Risk Prevention and Emergency Disposal South China University of TechnologyGuangzhou 510006China

Waste resource utilization of petroleum coke is crucial for achieving global carbon emission reduction.Herein,a series of N-doped microporous carbons were fabricated from petroleum coke using a One-pot synthesis method.The as-prepared samples had a large specific surface area(up to 2512 m^(2)/g),a moderate-high N content(up to 4.82 at.%),and high population(55%)of ultra-micropores(synthesis,primarily due to the existence of ultra-micropores.The sample exhibited excellent CO_(2)/N_(2)selectivity at 25℃ owing to the abundant basic pyridinic and pyrrolic N species;and showed superior CO_(2)adsorption-desorption cycling performance,which was maintained at 97% after 10 cycles at 25℃.Moreover,petroleum coke-based microporous carbon,with a considerably high specific surface area and hierarchical pore structure,exhibited excellent electrochemical performance over the N-doped sample,maintaining a favorable specific capacitance of 233.25F/g at 0.5 A/g in 6 mol/L KOH aqueous electrolyte.This study provides insight into the influence of N-doping on the porous properties of petroleum coke-based carbon.Furthermore,the as-prepared carbons were found to be promising adsorbents for CO_(2)adsorption,CO_(2)/N_(2)separation and electrochemical application.

关键词： One-pot synthesis N-doped microporous carbon CO_(2)adsorption CO_(2)/N_(2)selectivity Electrochemical performance

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One-pot synthesis of bimetallic CeCu-SAPO-34 for high-efficiency selective catalytic reduction of nitrogen oxides with NH_(3) at low temperature

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Chinese Journal of Chemical Engineering 2023年第4期56卷 193-202页

作者： Shuang Qiu Yonghou Xiao Haoran Wu Shengnan Lu Qidong Zhao Gaohong He Panjin Institute of Industrial Technology Liaoning Key Laboratory of Chemical Additive Synthesis and SeparationDalian University of TechnologyPanjin 124221China State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyPanjin 124221China School of Petrochemical Engineering Shenyang University of TechnologyLiaoyang 111003China

NH_(3) selective catalytic reduction(SCR) has been widely recognized as a promising technique for reducing nitrogen oxides from diesel vehicle exhausts. High-efficiency SCR catalysts that could perform at low temperatures are essential to denitration. In this work, a series of bimetallic CeCu-SAPO-34 molecular sieves were synthesized by one-step hydrothermal method. The Ce Cu-SAPO-34 maintained good crystallinity and a regular hexahedron appearance of Cu-SAPO-34 after introducing Ce species, while exhibiting a higher specific surface area and pore volume. The as-prepared CeCu-SAPO-34 with 0.02%(mass) Ce constituent exhibited the best catalytic activity below 300℃ and a maximum NO_(x) conversion of 99% was attained;the NO_(x) removal rates of more than 68% and 94% were achieved at 150℃ and 200℃, respectively. And the introduction of cerium species in Cu-SAPO-34 improves the low-temperature hydrothermal stability of the catalyst towards NH_(3)-SCR reaction. Additionally, the introduced Ce species could enhance the formation of abundant weak Br?nsted acid centers and promote the synergistic effect between CuO grains and isolated Cu^(2+) to enhance the redox cycle, which benefit the NH_(3)-SCR reaction.This work provides a facile synthesis method of high-efficiency SCR denitration catalysts towards diesel vehicles exhaust treatment under low temperature.

关键词： CeCu-SAPO-34 Selective catalytic reduction(SCR) Low temperature DeNO_(x) One-pot synthesis

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Radiation-induced One-pot synthesis of grafted covalent organic frameworks

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Science China Chemistry 2023年第6期66卷 1781-1787页

作者： Mingxing Zhang Mengjia Yuan Xiaofang Zhao Junchang Chen Linwei He Qianhong Gao Jiangtao Hu Guozhong Wu Zhifang Chai Shuao Wang State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201800China School of Environmental and Biological Engineering Nanjing University of Science&TechnologyNanjing 210094China

Post-synthetic functionalization of covalent organic frameworks(COFs)is an alternative way to enhance and broaden their properties and potential applications.However,the chemical functionalization of COFs is a great challenge because traditional procedures are often time-and energy-consuming,while the crystallinity of COFs can be damaged under harsh conditions.Here we report the in-situ introduction of functional graft chains onto the skeleton of COFs during the synthesis process through the combination of radiation-induced synthesis and graft polymerization techniques under ^(60)Co gamma-ray radiation.The synthesis and functionalization of COFs are simultaneously accomplished in a chemical system under ambient conditions yielding a large number of different functionalized COFs.The obtained carboxyl-functionalized COFs exhibit excellent radioactive uranium removal capabilities from aqueous solution with fast uptake dynamics,high adsorption capacity,and excellent selectivity over other competing metal ions.

关键词： covalent organic frameworks gamma ray radiation One-pot synthesis grafting functionalization uranium adsorption

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One-pot synthesis of CNT-SAPO-34 composite supported copper and cerium catalysts with excellent surface resistance to SO_(2) and H_(2)O in NH_(3)-SCR

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稀土学报:英文版 2023年第9期41卷 1344-1352,I0003页

作者： Yuanyuan Ma Zhifang Li Nan Zhao Mingyuan Shi Yuhang Sun Zheng Nan Liying Wang College of Chemistry and Chemical Engineering Qiqihar UniversityQiqihar 161006China College of Materials Science and Engineering Qiqihar UniversityQiqihar 161006China Analyzing&Testing Center Qiqihar UniversityQiqihar 161006China

CuCe/CNT_(x)-SAPO-34(x=0,0.5,1,2) with various CNT doping quantities were synthesized through the one-pot hydrothermal synthesis method using CNT and SAPO-34 as composite supporters.The selected CuCe/CNT_1-SAPO-34 catalyst exhibits remarkable SCR activity and high H_(2)O/SO_(2) resistance in a wide temperature range of 200-450℃.X-ray diffraction(XRD),N_(2) adsorption-desorption,scanning electron microscopy(SEM),X-ray photoelectro n spectroscopy(XPS),H_(2)-temperature programmed reduction(H2-TPR),and NH3-temperature programmed desorption(NH_(3)-TPD) were used to characterize the physiochemical structure,surface state of active sites reducibility,and surface acidity of the catalysts.The characterization results reveal that CuCe/CNT_1-SAPO-34 possesses a hierarchical structure,small particle size,high levels of surface Cu^(2+),Ce^(3+) and chemisorbed oxygen,enhanced reducibility,and suitable surface acidity.For comparison,CuCe/CNT_1-SAPO-34(P) mixed mechanically with CuCe/CNT_0-SAPO-34and CNT was investigated through the NH3-SCR with and without H_(2)O/SO_(2),it also displays lower resistance of H_(2)O and SO_(2) than CuCe/CNT_1-SAPO-34.The catalytic performance made CuCe/CNT_1-SAPO-34 a promising catalyst for the NO_(x) emission control from diesel vehicles.

关键词： CNT-SAPO-34 NH_(3)-SCR Copper(Cu) Cerium(Ce) One-pot synthesis Resistance to H_(2)O and SO_(2)

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Enhancing oxygen reduction reaction of Pt-Co/C nanocatalysts via synergetic effect between Pt and Co prepared by One-pot synthesis

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Rare Metals 2023年第1期42卷 146-154页

作者： Yun-Feng Wu Ji-Wei Ma Yun-Hui Huang School of Materials Science and Engineering Tongji UniversityShanghai201804China School of Materials Science and Engineering Huazhong University of Science and TechnologyWuhan430074China

Designing highly active and durable electrocatalysts towards oxygen reduction reaction(ORR)plays a paramount importance for proton exchange membrane fuel cells.Pt-based binary alloys Pt-M(M=3d-transition metals)possessing excellent electronic and geometric properties have received increasing interests as highly active electrocatalysts.Herein,we report a series of Pt_(x)Co/C(x=1,2,3)catalysts by a facile one-pot soft-chemistry method.In the acidic conditions,the mass activities of PtCo/C,Pt_(2)Co/C and Pt_(3)Co/C are 0.526,0.462 and 0.441 A·mgPt^(-1),which are 2.60,2.31 and 2.22 times higher than that of Pt/C(0.200 A·mgPt^(-1)),respectively.The specific activities of PtCo/C,Pt_(2)Co/C and Pt_(3)Co/C are 706.59,679.41 and 801.83μA·cm^(-2),which are accordingly 2.89,2.76 and 3.28 times higher than that of Pt/C(244.75μA·cm^(-2)).Notably,Pt_(3)Co/C shows a remarkable durability.After 5000 cycles of the accelerated durability testing,the mass activity and specific activity of Pt_(3)Co/C catalyst are 2.47 and 3.80 times higher than that of the commercial Pt/C,respectively.The improved ORR activity and durability can be ascribed to the synergistic interaction between Pt and Co.

关键词： Proton exchange membrane fuel cells(PEMFCs) Pt_(x)Co/C catalysts Synergetic effect Oxygen reduction reaction(ORR) One-pot synthesis

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One-pot synthesis of Fully-Conjugated Chemically Stable Two-Dimensional Covalent Organic Framework

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Chinese Journal of Chemistry 2022年第6期40卷 699-704页

作者： Hui Liu Yuxi Han Xuhan Zheng Jinyu Zhao Yixiao Man Lishui Sun Yingjie Zhao Engineering Research Center of High Performance Polymer and Molding Technology Ministry of EducationCollege of Polymer Science and EngineeringQingdao University of Science and TechnologyQingdaoShandong 266000China School of Materials Science and Engineering Shandong University of Science and TechnologyQingdaoShandong 266590China

Covalent organic frameworks(COFs)with good chemical stability coupled with extended-conjugation structures are highly prefera-ble.Herein,a fully-conjugated and chemically stable two-dimensional COF was synthesized by a one-pot,three-components synthe-sis through a successful conversion of amine,aldehyde,and alkyne groups into the quinoline units as linkages with B(C6F5)3 serving as a Lewis acid catalyst,whilst 2,3-dichloro-5,6-dicyano-1,4-benzoquinone(DDQ)was employed as an oxidant.The obtained fully conjugated 2D COF shows excellent stability in acid or base.

关键词： Covalent organic frameworks Fully-conjugated system Two-dimensional materials One-pot synthesis Chemical stability

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One-pot synthesis of Fe/Cu-SSZ-13 catalyst and its highly efficient performance for the selective catalytic reduction of nitrogen oxide with ammonia

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Journal of Environmental Sciences 2021年第2期33卷 306-316页

作者： Jie Wan Jiawei Chen Ru Zhao Renxian Zhou Energy Research Institute Nanjing Institute of TechnologyNanjing 211167China Institute of Catalysis Zhejiang UniversityHangzhou 310028China

Series of Fe/Cu-SSZ-13 catalysts with different Fe loading content were synthesized by simple one-pot strategy.The obtained catalysts were subjected to selective catalytic reduction(SCR)of NO x with NH 3 and were characterized by various techniques.The results show that Fe 0.63/Cu 1.50-SSZ-13 catalyst with proper Fe content exhibits excellent catalytic activity with widest operation temperature window from 160 to 580℃,excellent hydrothermal stability as well as good resistance to sulfur poisoning when compared with Cu-SSZ-13,signifying its great potential for practical applications.Further characterizations reveal that the synthesized Fe/Cu-SSZ-13 catalysts present typical chabazite(CHA)structure with good crystallinity,while isolated Cu^2+and monomeric Fe 3+are revealed as the predominant copper and iron species.At low temperatures,isolated Cu^2+species act as primary active sites for SCR reaction,while monomeric Fe^3+species provide sufficient active sites for sustain the SCR activity at high temperature.Moreover,Fe over doping would lead to the damage of zeolite structure,destruction of isolated Cu^2+site,as well as the formation of highly oxidizing Fe2O3,thus causing deterioration of catalytic performances.

关键词： NH3-SCR Fe/Cu-SSZ-13 One-pot synthesis Active species

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Facile One-pot synthesis of a novel all-carbon stair containing dimerized pentalene core from alkyne

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Chinese Chemical Letters 2022年第4期33卷 2047-2051页

作者： Hui Zhao Rakesh Kumar Gupta Wei Zhang Jiong Jia Qun Yu Zhiyong Gao Guilin Zhuang Dacheng Li Xingpo Wang Chen Ho Tung Di Sun Key Laboratory of Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringState Key Laboratory of Crystal MaterialsShandong UniversityJi’nan 250100China College of Chemical Engineering and Materials Science Zhejiang University of TechnologyHangzhou 310032China School of Chemistry and Chemical Engineering Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsKey Laboratory of Green Chemical Media and ReactionsMinistry of EducationHenan Normal UniversityXinxiang 453007China Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology and School of Chemistry and Chemical EngineeringLiaocheng UniversityLiaocheng 252000China

The construction of all-carbon molecule frameworks remains challenging. Herein, we report a facile and efficient One-pot synthesis of a novel all-carbon stair containing dimerized pentalene core using inexpensive cyclopropyl alkyne catalyzed by in situ generated Cu(I) from the comproportionation reaction of Cu(II) salt and Cu powder under mild reaction conditions. The reaction proceeds via sequential acetylenic coupling, followed by cyclization and [2 + 2] cycloaddition to directly produce pentalene dimer, which is difficult to access by other established methods. Different mechanistic paths were studied for the pentalene formation using density functional theory, suggesting that the reaction also proceeds through acetylenic coupling followed by cyclization and [2 + 2] cycloaddition. Based on the activation energy barriers, Path 1 has the rate-determining step of 38.63 kcal/mol, which is the most thermodynamically preferred one among the four paths.

关键词： One-pot synthesis Penatlene dimerization Comproportionation reaction Crystal structure Theoretical calculations

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One-pot synthesis of the highly efficient bifunctional Ni-SAPO-11 catalyst

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Journal of Materials Science & Technology 2021年第17期76卷 86-94页

作者： Yuchao Lyu Weilong Zhan Zhumo Yu Xinmei Liu Ye Yang Xiaoxing Wang Chunshan Song Zifeng Yan State Key Laboratory of Heavy Oil Processing China University of PetroleumQingdao 266580China EMS Energy Institute Pennsylvania State UniversityUniversity ParkPA16802USA

Hydro isomerization of linear alkanes to branched isomers is an important petrochemical process for production of gasoline with high octane number.Non-noble metal bifunctional catalysts used in this process always suffer from low metal dispersion and poor metal-acid synergy.Herein,a facile One-pot synthesis method was used to simultaneously regulate metal particle sizes and acidity of the Ni-SAPO-11 hydroisomerization catalyst.The physicochemical properties are investigated using XANES,EXAFS,TEM/STEM,FT-IR,XPS,UV-vis and NH_3-TPD.Apart from the highly dispersed nickel nanoparticles with an average diameter of 8 nm,the framework Ni~(2+)ions are generated via substituting framework Al~(3+)ions of the SAPO-11.The formed NiP-OH structures have lower deprotonation energy(DPE)than the SiAl-OH ones,contributing more and stronger acid sites to the Ni-SAPO-11 catalyst.The great metal-acid synergy including high metal to acid sites ratio(n_(Ni)/n_A)and close intimacy is obtained for the Ni-SAPO-11 catalyst.The Ni-SAPO-11 catalyst outperforms the counterpart prepared by the impregnation method and exhibits comparable activity and isomers selectivity to the Pt/SAPO-11 catalyst in the n-hexane hydroisomerization.

关键词： One-pot synthesis Nickel SAPO-11 Hydroisomerization Metal-acid synergy

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One-pot synthesis of Cu-Ce co-doped SAPO-5/34 hybrid crystal structure catalysts for NH_(3)-SCR reaction with SO_(2) resistance

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Journal of Rare Earths 2021年第10期39卷 1217-1223,I0002页

作者： Yuanyuan Ma Zhifang Li Nan Zhao Yanlong Teng College of Chemistry and Chemical Engineering Qiqihar UniversityQiqihar 161006China College of Materials Science and Engineering Qiqihar UniversityQiqihar 161006China Analyzing&Testing Center Qiqihar UniversityQiqihar 161006China

SAPO-34,SAPO-5/34 based catalysts doped with Cu,Ce as active components were synthesized via a one-pot hydrothermal method by using different amounts of additive(a-cellulose),and their catalytic activities were measured for selective catalytic reduction(SCR) of NO with NH3.The synthesized Cu-Ce co-doped products switch from cubic SAPO-34,to flower-like aggregated SAPO-5/34,hybrid crystal SAPO-5/34,and finally to spherical aggregated SAPO-34 with the increase of α-cellulose amount.The Cu-Ce co-doped SAPO-5/34 hybrid crystal structure catalysts with 0.75 mol ratios of C/P(Cu-Ce/SP-0.75)exhibit excellent NH_(3)-SCR activity with higher than 90% NOx conversion in the temperature range of 180-450℃,at WHSV of 20000 mL/(g·h).Furthermore,the catalyst displays outstanding sulfur resistance and NOX conversion maintains above 90% at 200-450℃ after adding 100 ppm of SO_(2).The characteristic results suggest that the high deNOX performance of Cu-Ce/SP-0.75 is due to the enhanced accessibility,abundant activity species,excellent redox property and high adsorptive and activated capacity for NH_(3).

关键词： SAPO-5/34 catalysts Selective catalytic reduction Cu-Ce co-modified One-pot synthesis Good resistance to SO_(2) Rare earths

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