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Exploration of the interaction mechanism in the synergistic degradation of benzene and toluene over MnCoOx catalysts

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Frontiers of Environmental Science & engineering 2025年第2期19卷 119-134页

作者： Xin Xing Zhe Li Yixin Wang Zonghao Tian Jie Cheng Zhengping Hao College of Environment and Resources Taiyuan University of Science and TechnologyTaiyuan 030024China National Engineering Laboratory for VOCs Pollution Control Material&Technology Research Center for Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China

The catalytic degradation of single-component vocs has been widely ***,several types of vocs may be present in an actual industrial emission *** synergistic removal of multicomponent vocs is currently a popular research ***,Mn–Co samples with various Mn/Co ratios(1:2,1:1,and 2:1)were successfully prepared,and the catalytic oxidation performance characteristics toward benzene and toluene over these samples under single and binary VOC oxidation conditions were *** with pure MnOx and CoOx,the prepared Co–Mn composite oxide samples exhibited significantly improved catalytic *** and MnCo2Ox showed optimum catalytic performance,with 100%benzene and 100%toluene conversion in the mixtures at 300 and 350°C,100%CO_(2) *** methods were employed to elucidate the relevance of the catalytic activity to the structures,acidity,redox properties,Mn–Co valence state and oxygen ***,the interactions between benzene and toluene during their synergistic degradation,as well as the intermediates and potential reaction mechanisms of their simultaneous elimination,were *** Mn–Co oxide compounds for cooperative catalytic oxidation of benzene and toluene represents a viable and effective technique for the practical and synergist elimination of multicomponent vocs.

关键词： Mn-Co oxides Synergetic catalytic oxidation Benzene and toluene Reaction mechanism

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CeO_(2)@MnO_(2)with strong Ce-Mn interaction activating PDS to promote in situ degradation of adsorbed tetracycline

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Journal of Rare Earths 2025年第3期43卷 490-499,I0003页

作者： Jinhui Zhang Jiawei Sun Xinfeng Zhu Jingquan Liu Linlin Chang Guofeng Li Rongfu Peng Junning Wang Libin Jiang Kai Wang Shiqiang Yin Xueping Liu Chaohai Wang Henan Key Laboratory of Water Pollution Control and Rehabilitation Technology School of Municipal and Environmental EngineeringHenan University of Urban ConstructionPingdingshan467036China National Engineering Laboratory for voCs Pllution Control Technology and Equipment Guangzhou510006China School of Light Industry&Chemical Engineering Dalian Polytechnic UniversityDalian116034China

A series of CeO_(2)@MnO_(2)composites was prepared by deposition-precipitation *** materials were used to activate sodium persulfate(PDS)for the oxidation of *** is found that the composites,especially the CeO_(2)@MnO_(2)-1:4 composites,exhibit better tetracycline removal rates than the pure components.X-ray diffraction(XRD),Raman and scanning electron microscopy(SEM)analyses all indicate that the composite has been successfully prepared with high purity and high *** XPS analysis shows that the strong interaction between the components promotes the electron ***,the kinetic rate constants of CeO_(2)@MnO_(2)-1:4 after 60 min are 3.8 and 12.7 times higher than pure CeO_(2)and MnO_(2),***_(2)@MnO_(2-)1:4 composite also exhibits excellent catalytic activity for individual and hybrid *** effects of wastewater matrix,pH,circulation and ion stre ngth on the degradation of tetracycline were *** is found that CeO_(2)@MnO_(2)-1:4 composite has good practical application ***_(2)@MnO_(2)composites with synergistic adsorption catalysis can activate PDS and peroxymo no sulfate(PMS)for efficient organic catalytic *** paper provides the theoretical basis and data support for the practical application of the CeO_(2)@MnO_(2)composite materials.

关键词： Tetracycline Multicomponent contamination Adsorption-catalytic synergy Anti-interference CeO_(2)@MnO_(2) Rare earths

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Insight into catalytic performance and reaction mechanism for toluene total oxidation over Cu-Ce supported catalyst

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Journal of Environmental Sciences 2025年第3期149卷 476-487页

作者： Xuan Liang Jin Zhang Juntai Tian Zenghua Xie Yue Liu Peng Liu 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 South China University of TechnologyGuangzhou 510006China Guangdong Provincial Engineering and Technology Research Centre for Environmental Risk Prevention and Emergency Disposal South China University of TechnologyGuangzhou 510006China

Herein,three supported catalysts,CuO/Al_(2)O_(3),CeO_(2)/Al_(2)O_(3),and CuO-CeO_(2)/Al_(2)O_(3),were synthesized by the convenient impregnation method to reveal the effect of CeO_(2)addition on catalytic performance and reaction mechanism for toluene *** with CuO/Al_(2)O_(3),the T_(50)and T_(90)(the temperatures at 50%and 90%toluene conversion,respectively)of CuO-CeO_(2)/Al_(2)O_(3)were reduced by 33 and 39°C,respectively.N_(2)adsorptiondesorption experiment,XRD,SEM,EDS mapping,Raman,EPR,H_(2)-TPR,O_(2)-TPD,XPS,NH_(3)-TPD,Toluene-TPD,and in-situ DRIFTS were conducted to characterize these *** excellent catalytic performance of CuO-CeO_(2)/Al_(2)O_(3)could be attributed to its strong coppercerium interaction and high oxygen vacancies ***,in-situ DRIFTS proved that CuO-CeO_(2)/Al_(2)O_(3)promoted the conversion of toluene to benzoate and accelerated the deep degradation path of *** work provided valuable insights into the development of efficient and economical catalysts for volatile organic compounds.

关键词： Cu-Ce supported catalyst Copper-cerium interaction Oxygen vacancies Toluene oxidation Reaction mechanism

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Surface reaction-induced LaBO3 nano-islands confine dispersed Ni species for highly efficient NH3 decomposition

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Applied Catalysis A: General 2025年 699卷

作者： Yang, Zhenwen Shui, Ziyi Niu, Ben Duan, Xiaoxiao Wei, Zheng Jiang, Guoxia Hao, Zhengping Research Center for Environmental Material and Pollution Control Technology National Engineering Laboratory for VOCs Pollution Control Material & Technology University of Chinese Academy of Sciences Beijing101408 China

NH3 decomposition is receiving increased attention for on-site COx-free H2 generation. Unfortunately, the harsh reaction conditions often cause sintering of active metals. Here we report a simple method to achieve well Ni dispersion by nano-structuring the BN support with La species. The surface reaction-induced LaBO3 nano-islands on BN support have a strong affinity for Ni atoms, which can capture and confine Ni species to yield a large population of well dispersed Ni clusters and nanoparticles. The Ni species selectively anchored on LaBO3 islands expose more active sites and boost desorption of N2 and H2, exhibiting superior activity and stability for NH3 decomposition. In addition, it is revealed that the Ni dispersion is sensitive to the change of the support surface structure. These findings highlight the important role of support structure in determining the nature of the metal phase and provide guidance for designing catalysts with controlled catalytic structure and reactivity. © 2025 Elsevier B.V.

关键词： Surface reactions

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Highly efficient and stable single-atom Cu encapsulated in silicalite-1 zeolite for selective catalytic oxidation of nitrogen-containing vocs

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Applied Catalysis B: Environmental 2025年 371卷

作者： Zhao, Ting Niu, Ben An, Weiqi Li, Bingzhi Li, Ganggang Shui, Ziyi Duan, Xiaoxiao Zhang, Zhongshen Cheng, Jie Hao, Zhengping National Engineering Laboratory for VOCs Pollution Control Material & Technology Research Center for Environmental Material and Pollution Control Technology University of Chinese Academy of Sciences Beijing101408 China New Energy Technology Research Institute CHN Energy Beijing102209 China

The urgent need to eliminate highly hazardous nitrogen-containing volatile organic compounds (Nvocs) necessitates the development of catalysts that exhibit exceptional activity, N2 selectivity, and stability. Herein, single-atom Cu encapsulated in silicalite-1 zeolite (Cu1@S-1) was prepared and comprehensively compared with Cu/S-1and Cun@S-1 in the selective catalytic oxidation of Nvocs. The results of integrated differential phase contrast scanning transmission electron microscopy (iDPC-STEM), X-ray absorption spectroscopy (XAS), ultraviolet-visible-near infrared spectroscopy (UV-Vis-NIR), and nuclear magnetic resonance spectroscopy (NMR) revealed that the isolated Cu with the {([tbnd]SiO)2Cu(HO−Si[tbnd])2} structure embedded into the T1(7) and T3(9) sites of S-1 zeolites in Cu1@S-1. These well-defined Cu active sites collaborate with the zeolite-confined microenvironment to enhance oxygen activation, generate appropriate surface acidity, and facilitate the transformation of reactive intermediate species. Consequently, Cu1@S-1 demonstrates excellent catalytic performances for selective catalytic oxidation of n-butylamine, achieving T100 at 280°C and 92 % N2 selectivity at 100 % (CO+CO2) yield, thus surpassing Cun@S-1 and Cu/S-1. Furthermore, the isolated Cu sites in Cu1@S-1 exhibit high resistance to sintering even after hydrothermal treatment at 700°C. This work provides crucial insights for the environmentally friendly destruction of Nvocs via developing active and stable single-atom Cu encapsulated in zeolite catalysts. © 2025

关键词： Nuclear magnetic resonance spectroscopy

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In-situ engineering of Amine-Functionalized layered double hydroxide nanosheets for highly enhanced efficiency in direct air capture of CO2

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Separation and Purification technology 2025年 367卷

作者： Jin, Yi Chen, Xinyu Ma, Fengying Leng, Jinhai Wu, Jianqing Yu, Miao Huang, Haomin Shang, Shanshan Ye, Daiqi Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control National Engineering Laboratory for VOCs Pollution Control Technology and Equipment School of Environment and Energy South China University of Technology Guangzhou510006 China

The development of amine-functionalized adsorbents represents a significant advancement in direct air capture (DAC) technologies for carbon dioxide (CO2) mitigation. Layered double hydroxides (LDHs) offer numerous benefits for DAC applications, including abundant adsorption sites, cost-effectiveness, and alkali resistance, making them ideal for amine loading. However, the conventional impregnation method (C-Im) leads to reduced surface area and platelet aggregation, impeding amine uniform dispersion. This study introduces a novel aqueous miscible organic solvent impregnation method (A-Im) for the in-situ loading of three alkyl primary diamines onto magnesium (Mg) and aluminum (Al)-based LDHs. CO2 adsorption isotherms demonstrated that the amine-functionalized LDHs synthesized via A-Im (LDH-A-AM) significantly outperformed C-Im counterparts (LDH-C-AM), with LDH-A-EDA achieving the highest CO2 adsorption capacity of 0.80 mmol/g at 0.4 mbar and 2.71 mmol/g at 1.0 bar, representing 40 and 8.7 times higher capacities, respectively, than that of LDH-C without amine. Adsorption kinetic studies revealed a rapid adsorption rate of 0.052 mmol/(g·min) and an impressive regeneration performance of 86 % after 10 cycles. Under humid conditions, CO2 breakthrough experiments demonstrated that LDH-A-EDA possessed enhanced CO2 adsorption capacities across varying relative humidity (0–75 %). The DAC mechanism elucidated that LDH-A-AM adsorbed CO2 via both physisorption and chemisorption by enhanced –OH and –NH2 sites. These findings position LDHs as effective carriers for amines, advancing CO2 capture technologies and contributing to sustainable climate solutions. © 2025 Elsevier B.V.

关键词： Direct air capture

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Chromium Promoted the Efficient and Stable Catalytic Degradation of Propane Over Pt/Hzsm-5 Catalyst: Optimization and Reaction Mechanism

SSRN

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SSRN 2025年

作者： Jian, Yanfei Xu, He Wang, Yao Wang, Jingjing Xia, Lianghui Liu, Yujie Yu, Yanke He, Chi State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power Engineering Xi'an Jiaotong University Shaanxi Xi'An710049 China National Engineering Laboratory for VOCs Pollution Control Material and Technology University of Chinese Academy of Sciences Beijing101408 China Yunnan University China

Light alkanes are a class of ubiquitous volatile organic compounds (vocs), which bring great environmental hazards and health risks. However, low-temperature degradation of light alkanes is still a great challenge. Herein, a series of Pt/HZSM-5 catalysts without/with additives of Cr were fabricated. Catalytic performance of the catalyst for C3H8 low temperature combustion was investigated. It was found that Cr element had a significant effect on the activity of Pt/HZSM-5. Pt/Cr1/HZSM-5 performed the best activity for C3H8, excellent high temperature stability and water resistance. Characterization results of catalysts indicated that the introduction of Cr element could fix Pt site to promote the dispersion of Pt on the support. Moreover, the interaction between Cr and Pt produced more active Pt species, surface active lattice oxygen and acidic sites, which could promote the activation of C-H bonds in C3H8. Theoretical calculations showed that the interface between Pt and Cr had stronger adsorption for O2 and C3H8, which could accelerate propane oxidation. In this study, the effect of transition metal elements on the promotion of noble metal catalysts in the low-temperature degradation of light alkanes was discussed in depth, and it provided a reference for the design of efficient noble metal molecular sieve catalysts. © 2025, The Authors. All rights reserved.

关键词： Molecular sieves

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Effect of Cu-ZSM-5 catalysts with different CuO particle size on selective catalytic oxidation of N,N-Dimethylformamide

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Frontiers of Environmental Science & engineering 2022年第10期16卷 1-10页

作者： Xin Xing Na Li Dandan Liu Jie Cheng Zhengping Hao College of Environmental Science and Engineering Taiyuan University of Science and TechnologyTaiyuan 030024China National Engineering Laboratory for VOCs Pollution Control Material&Technology Research Center for Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China

N,N-Dimethylformamide(DMF),a nitrogen-containing volatile organic compound(NVOC)with high emissions from the spray industry,has attracted increasing *** this study,Cu-ZSM-5 catalysts with different CuO particle sizes of 3,6,9 and 12 nm were synthesized and tested for DMF selective catalytic *** crystal structure and physicochemical properties of the catalyst were studied by various characterization *** catalytic activity increases with increasing CuO particle size,and complete conversion can be achieved at 300-350℃.The Cu-12 nm catalyst has the highest catalytic activity and can achieve complete conversion at 300℃.The Cu-6 nm sample has the highest N_(2)selectivity at lower temperatures,reaching 95%at 300℃.The activity of the catalysts is determined by the surface CuO cluster species,the bulk CuO species and the chemisorbed surface oxygen *** high N_(2)selectivity of the catalyst is attributed to the ratio of isolated Cu2+and bulk CuO species,and weak acidity is beneficial to the formation of N_(2).The results in this work will provide a new design of NVOC catalytic oxidation catalysts.

关键词： N,N-Dimethylformamide Selective catalytic oxidation Cu-ZSM-5 CuO particle size

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A review of whole-process control of industrial volatile organic compounds in China

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Journal of Environmental Sciences 2023年第1期123卷 127-139页

作者： Hailin Wang Shumei Sun Lei Nie Zhongshen Zhang Wenpeng Li Zhengping Hao Beijing Key Laboratory for Urban Atmospheric VOCs Pollution Control and Technology Application Beijing Municipal Research Institute of Environmental ProtectionBeijing 100037China College of Resources Environment and Tourism Capital Normal UniversityBeijing 100048China National Engineering Laboratory for VOCs Pollution Control Material&Technology Research Center for Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China

Volatile organic compounds(vocs)play an important role in the formation of ground-level ozone and secondary organic aerosol(SOA),and they have been key issues in current air pollution prevention and control in *** attention has been paid to industrial activities due to their large and relatively complex vocs *** present research aims to provide a comprehensive review on whole-process control of industrial vocs,which mainly includes source reduction,collection enhancement and end-pipe *** vocs materials including water-borne ones are the keys to source substitution in industries related to coating and solvent usage,leak detection and repair(LDAR)should be regarded as an efficient means of source reduction in refining,petrochemical and other chemical *** types of vocs collection methods such as gas-collecting hoods,airtight partitions and others are discussed,and airtight collection at negative pressure yields the best collection *** end-pipe treatments like UV oxidation,low-temperature plasma,activated carbon adsorption,combustion,biodegradation,and adsorption-combustion are discussed in ***,several recommendations are made for future advanced treatment and policy development in industrial vocs emission control.

关键词： Volatile organic compounds materials substitution Collection enhancement End-pipe treatments

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Promotional effect of Cu additive for the selective catalytic oxidation of n-butylamine over CeZrO_(x)catalyst

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Chinese Chemical Letters 2022年第6期33卷 3065-3072页

作者： Xin Xing Ting Zhao Jie Cheng Xiaoxiao Duan Wenpeng Li Ganggang Li Zhongshen Zhang Zhengping Hao National Engineering Laboratory for VOCs Pollution Control Material&Technology Research Center for Environmental Material and Pollution Control TechnologyUniversity of Chinese Academy of SciencesBeijing 101408China College of Environmental Science and Engineering Taiyuan University of Science and TechnologyTaiyuan 030024China

The catalytic elimination of nitrogen-containing volatile organic compounds(Nvocs)still encounters bottlenecks in NO_(x)formation and low N_(2)***,a series of Cu-promoted Ce-Zr mixed oxide catalysts were synthesized using a simple precipitation approach,and n-butylamine was adopted as the probe pollutant to evaluate their catalytic *** Ce Cu_(10%)ZrO_(x)catalyst exhibited the best catalytic activity,with 100%n-butylamine conversion and 90%N_(2)selectivity at 250℃.Concurrently,this sample also displayed good water resistance.A detailed characterization of the catalyst was performed through a series of experimental studies and theoretical *** addition of Cu increased the redox property and promoted the production of oxygen vacancies,all of which were favorable for the greatest nbutylamine selective catalytic oxidation *** changes of oxygen vacancies over Ce Cu_(10%)ZrO_(x)in reaction process were studied by in situ Raman ***,in situ diffuse reflectance infrared Fourier transform spectra(DRIFTs)and theoretical calculations were employed to explore the reaction mechanism of n-butylamine selective *** high activity and selectivity of this catalyst confirm the practical feasibility of the selective oxidation of n-butylamine to CO_(2)and N_(2),and the exploration of the reaction mechanism provides new insights into the further design of catalysts.

关键词： N-Butylamine CeCu_(a)ZrO_(x)mixed oxide Selective oxidation Oxygen vacancies Reaction mechanism

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