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Enhanced photocatalytic activity of rGO/TiO2 for the decomposition of formaldehyde under visible light irradiation

Journal of Environmental Sciences 2018年第11期30卷 138-146页

作者： Lian Yu Long Wang Xibo Sun Daiqi Ye College of Environment and Energy South China University of Technology Guangzhou 510006 China Cuangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control Guangzhou 510006 China National Engineering Laboratory for VOCs Pollution Control Technology and Equipment South China University of Technology Guangzhou 510006 China

Due to the low concentration of indoor air contaminants, photocatalytic technology shows low efficiency for indoor air purification. The application of TiO2 for photocatalytic removal of formaldehyde is limited, because TiO2 can only absorb ultraviolet （UV） light. Immobilization of TiO2 nanoparticles on the surface of graphene can improve the visible light photocatalytic activity and the adsorption capacity. In this study, rGO （reduced graphene oxide）/TiO2 was synthesized through a hydrotherrnal method using titanium tetrabutoxide and graphene oxide as precursors, and was used for the degradation of low concentration formaldehyde in indoor air under visible light illumination. Characterization of the crystalline structure and morphology of rGO/TiO2 revealed that most GO was reduced to rGO during the hydrothermal treatment, and anatase TiO2 nanoparticles （with particle size of 15-30 nm） were dispersed well on the surface of the rGO sheets, rGO/TiO2 exhibited excellent photocatalyfic activity for degradation of formaldehyde in indoor air and this can be attributed to the role ofrGO, which can act as the electron sink and transporter for separating photo-generated electron-hole pairs through interfacial charge transfer. Furthermore, rGO could adsorb formaldehyde molecules from air to produce a high concentration of formaldehyde on the surface of rGO/ TiO2. Under visible light irradiation for 240 min, the concentration of formaldehyde could be reduced to 58.5 ppbV. rGO/TiO2 showed excellent moisture-resistance behavior, and after five cycles, rGO/TiO2 maintained high photocatalytic activity for the removal of formaldehyde （84.6%）. This work suggests that the synthesized rGO/TiO2 is a promising photocatalyst for indoor formaldehyde removal.

关键词： Reduced graphene oxide （rGO） rGO/TiO2 nanocomposites Visible light photocatalysis Indoor air Formaldehyde

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Utilization of steelwork off-gases through methanol synthesis: Sulfur-induced dynamic migration of ZnO x over industrial Cu/ZnO/Al 2 O 3 catalyst and the poisoning mechanism

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Journal of Environmental Sciences 2025年

作者： Yukun Tian Yu Zeng Ziyang Chen Hua Tong Ming Chen Zhiyong Zhong Daiqi Ye Limin Chen Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control School of Environment and Energy South China University of Technology Guangzhou 510006 China National Engineering Laboratory for VOCs Pollution Control Technology and Equipment South China University of Technology Guangzhou 510006 China The Key Lab of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of Education South China University of Technology Guangzhou 510006 China

The reduction of carbon emissions in the steel industry is a significant challenge, and utilizing CO 2 from carbon intensive steel industry off-gases for methanol production is a promising strategy for decarbonization. However, steelwork off-gases typically contain various impurities, including H 2 S, which can deactivate commercial methanol synthesis catalysts, Cu/ZnO/Al 2 O 3 (CZA). Reverse water-gas shift (RWGS) reaction is the predominant side reaction in CO 2 hydrogenation to methanol which can occur at ambient pressure, enabling the decouple of RWGS from methanol production at high pressure. Then, a series of activated CZA catalysts has been in-situ pretreated in 400 ppm H 2 S/Ar at 250 ℃ and tested for both RWGS reaction at ambient pressure and CO 2 hydrogenation to methanol at high pressure. An innovative decoupling strategy was employed to isolate the RWGS reaction from the methanol synthesis process, enabling the investigation of the evolution of active site structures and the poisoning mechanism through elemental analysis, X-ray Diffraction, X-ray Photoelectron Spectroscopy, Fourier Transform Infrared Spectroscopy, Temperature Programmed Reduction and CO 2 Temperature Programmed Desorption. The results indicate that there are different dynamic migration behaviors of ZnO x in the two reaction systems, leading to different poisoning mechanisms. These interesting findings are beneficial to develop sulfur resistant and durable highly efficient catalysts for CO 2 hydrogenation to methanol, promoting the carbon emission reduction in steel industry.

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Fabricating PdCe/OMS-2 catalysts with boosted low-temperature activity for toluene deep degradation

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Journal of Rare Earths 2023年第6期41卷 839-849,I0002页

作者： Lin Yue Zhihua Xu Minghua Hu Mingjiao Tian Mudi Ma Bijie Huang Chi He State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power EngineeringXi'an Jiaotong UniversityXi'an 710049China State Key Laboratory of Precision Blasting and Hubei Key Laboratory of Industrial Fume and Dust Pollution Control Jianghan UniversityWuhan 430056China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 101408China

Porous cryptomelane-type octahedral molecular sieve(OMS-2)with mixed Mn valence and abundant lattice oxygen species has attracted much attention in volatile organic compounds(VOC)catalytic ***,complete conversion of arene over OMS-2 catalysts at relatively low temperature is still a challenge due to its limited crystal structure and inferior ***,a series of PdCe/OMS-2 catalysts with different Pd/Ce molar ratios was fabricated by a facile impregnation method and the physicochemical properties of which were extensively characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),high-resolution transmission electron microscopy(HR-TEM),B runauer-Emmett-Teller(BET)method,X-ray fluorescence(XRF),X-ray photoelectron spectroscopy(XPS),temperature programmed reduction of H2(H2-TPR),Raman,In situ diffused reflectance infrared Fourier transform spectra(DRIFTS),and density functional theory(DFT)*** show that the total conversion of toluene can be achieved at 207℃ over PdCe2 with apparent activation energy as low as 62.6 kJ/*** strong synergistic effect between Pd and Ce remarkably boosts the catalytic activity of OMS-2,attributed to the abundant Mn^(3+)-O bands and active surface oxygen *** results reveal that oxygen vacancy can be formed over PdCe2 much easily than that of Pd/OMS-2 and Ce/OMS-2 with the oxygen vacancy formation energy of2.42,2.83 and 2.68 eV,*** increasing the Pd content cannot promote the catalytic activity although PdO is a critical active center in toluene *** vacancy attributed to the integrative effect of Pd,Ce and Mn species plays a promine nt role over prepared catalysts in toluene activation *** findings reported in this work showed new insights into the designing of highly efficient OMS-2catalysts for VOC deep oxidation by tuning oxygen vacancy concentration.

关键词： PdCe/OMS-2 Toluene Catalytic oxidation Oxygen vacancy Rare earths

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Decomposition of dioxin-like components in a DBD reactor combined with Hg/Ar electrodeless ultraviolet

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Plasma Science and technology 2020年第3期22卷 34-39页

作者： Weixuan ZHAO Liping LIAN Yanpei WU Yanghaichao LIU Renxi ZHANG Gang LUO Huiqi HOU Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Institute of Environmental ScienceFudan UniversityShanghai 200433People’s Republic of China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 100049People’s Republic of China

A new combined reactor with Hg/Ar electrodeless ultraviolet(EDUV)activated by DBD for 3,4-dichlorodiphenyl ether abatement is *** effect of specific input energy and feeding gas component on 3,4-dichlorodiphenyl ether removal efficiency has been *** with a single DBD system,this new combined process performed a significant promotion on 3,4-dichlorodiphenyl ether *** results verified that active oxygen clearly contributed to the synergistic activity of DBD-EDUV *** of emission spectra showed that UV radiation of 253.7 nm could be detected in the DBD-EDUV ***,the products of DBD-EDUV process were analyzed via gas chromatographymass spectrometer(GC-MS)to reveal involved decomposition mechanism.

关键词： dielectric barrier discharge(DBD) dioxin-like 3,4-dichlorodiphenyl ether EDUV photolysis

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DBD coupled with MnOx/γ-Al2O3 catalysts for the degradation of chlorobenzene

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Plasma Science and technology 2020年第3期22卷 115-122页

作者： Yanghaichao LIU Liping LIAN Weixuan ZHAO Renxi ZHANG Huiqi HOU Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Institute of Environmental ScienceFudan UniversityShanghai 200433People’s Republic of China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 100049People’s Republic of China

This paper investigates the degradation of chlorobenzene by dielectric barrier discharge(DBD)coupled with MnOx/γ-Al2O3 ***/γ-Al2O3 catalysts were prepared using the impregnation method and were characterized in detail by N2 adsorption/desorption,x-ray diffraction and x-ray photoelectron *** with the single DBD reactor,the coupled reactor has a better performance on the removal rate of chlorobenzene,the selectivity of COx,and the inhibition of ozone production,especially at low discharge *** degradation rate of chlorobenzene and selectivity of COx can reach 96.3%and 53.0%,respectively,at the specific energy density of 1350 J ***,the ozone concentration produced by the discharge is significantly reduced because the MnOx/Al2O3 catalysts contribute to the decomposition of ozone to form oxygen atoms for the oxidation of *** addition,based on analysis of the byproducts,the decomposition mechanism of chlorobenzene in the coupled reactor is also discussed.

关键词： plasma catalytsis system chlorinated vocs MnOx/Al2O3 catalysts

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Synergistic effect of oxygen vacancies and edging/corner-connected MnOs structural motifs in multi-dimensional manganese oxides to enhance Ovocs catalytic oxidation

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Chinese Chemical Letters 2023年第12期34卷 291-299页

作者： Yonggang Sun Ganggang Li Jie Cheng Na Li Xin Xing Xin Zhang Zhongshen Zhang State Key Laboratory of High-eficiency Coal Utilization and Green Chemical Engineering School of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021China 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 Resources and Environment University of Chinese Academy of SciencesBejing 101408China

The structure-activity relationships for vinyl acetate catalytic oxidation are challenging to explore at the atomic scale due to the ambiguity of the structural defect types and sites of manganese *** work elaborates,at the atomic level,through in-situ experimental and theoretical methods,the synergistic effects of two types of structural defect sites of Vo-e(edge-sharing oxygen)and Vo-c(corner-sharing oxygen)and MnO6 structural motifs of manganese ***-dimensional manganese oxides,namely those with corner-connected MnOs structural motifs and Vo-c structural oxygen defect sites,significantly improved the activation of vinyl *** of enol structure formation,acetate and formate intermediate species,and tautomerism between enol structure and acetaldehyde were detected when oxygen vacancies of manganese oxides were present in combination with corner/edge-connected ***,the activation of chemical bonds and deep catalytic oxidation of vinyl acetate depend on the presence of a redox couple,surface oxygen species,and weakened Mn-O *** provides a valuable notion for investigating and designing catalytic systems and reaction processes for the purpose of emission reduction and the management of environmental contaminants.

关键词： Oxygen vacancies Synergistic effects MnO_(6)structural motifs In-situ technologies Catalytic oxidation

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In situ electron-induced reduction of NOx via CNTs activated by DBD at low temperature

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Frontiers of Environmental Science & engineering 2020年第2期14卷 87-96页

作者： Weixuan Zhao Liping Lian Xingpeng Jin Renxi Zhang Gang Luo Huiqi Hou Shanping Chen Ruina Zhang Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3) Institute of Environmental ScienceFudan UniversityShanghai 200433China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 100049China Shanghai Institute for Design&Research on Environmental Engineering Shanghai 200232China

In this study,a new in situ electron-induced process is presented with carbon nanotubes(CNTs)as a reduction agent activated by dielectric barrier discharge(DBD)for nitrogen oxide(NOx)abatement at low temperature(<407 K).Compared with a single DBD system and a DBD system with activated carbon(DBD-AC),a DBD system with carbon nanotubes(DBD-CNT)showed a significant promotion of NOx removal efficiency and N2 *** the 02 content was 10%,the NOv conversion and N2 selectivity in the DBD-CNT system still reached 64.9%and 81.9%at a specific input energy(SIE)of 1424 J^L,and these values decreased to 16.8%,31.9%and 43.2%,62.3%in the single DBD system and the DBD-AC system,respectively.X-ray photoelectron spectroscopy(XPS)and scanning electron microscopy(SEM)were utilized to investigate surface changes in the CNTs after activation by DBD to explore the NO.t reduction abatement mechanism of this new ***,the outlet gas components were also observed via Fourier transform infrared spectroscopy(FTIR)to help reveal the NOr reduction *** results verified that carbon atoms excited by DBD and the structure of CNTs contributed to the synergistic activity of the DBD-CNT *** new deNOx process was accomplished through in situ heterogenetic reduction reactions between the NOx and carbon atoms activated by the plasma on the *** addition,further results indicated that the new deNOv process exhibited acceptable S02 tolerance and water resistance.

关键词： Dielectric barrier discharge NOx abatement In situ electron-induced reduction Carbon nanotubes

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Honeycomb-like biochar framework coupled with Fe_(3)O_(4)/FeS nanoparticles as efficient heterogeneous Fenton catalyst for phenol degradation

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Journal of Environmental Sciences 2024年第2期136卷 390-399页

作者： Aihua Cheng Yi He Xiaohe Liu Chi He Department of Environmental Engineering College of Geology and EnvironmentXi’an University of Science and TechnologyXi’an 710054China State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power EngineeringXi’an Jiaotong UniversityXi’an 710049China National Engineering Laboratory for VOCs Pollution Control Material and Technology University of Chinese Academy of SciencesBeijing 101408China

Achieving an efficient and stable heterogeneous Fenton reaction over a wide pH range is of great significance for wastewater ***,a pollen-derived biochar catalyst with a unique honeycomb-like structure,coupled with the dispersion of magnetic Fe_(3)O_(4)/FeS(Fe/S)nanoparticles,was synthesized by simple impregnation precursor,followed by *** prepared Fe/S-biochar catalyst demonstrated outstanding phenol degradation efficiency across a wide pH range,with 98%of which eliminated even under neutral conditions(pH 7.0).The high catalytic activity was due to the multilevel porous structure of pollenderived biochar provided enough active sites and allowed for better electron transfer,then increases oxidation ability to promote the ***,the acid microenvironment formed by SO_(4)^(2-)group from Fe/S composite extended the pH range for Fenton reaction,and S^(2-)facilitated the conversion of≡Fe^(3+)to≡Fe^(2+),resulting in remarkable degradation ***,biochar can effectively promote cycling stability by limiting Fe *** work may provide a general strategy for designing 3D framework biochar-based Fe/S catalysts with excellent performance for heterogeneous Fenton reactions.

关键词： Biomass Biochar Fenton reaction Fe_(3)O_(4)/FeS(Fe/S) Phenol degradation

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Efficient NO_x abatement by passive adsorption over a Pd-SAPO-34 catalyst prepared by solid-state ion exchange

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Chinese Chemical Letters 2024年第4期35卷 210-213页

作者： Linhui Liu Wuwan Xiong Mingli Fu Junliang Wu Zhenguo Li Daiqi Ye Peirong Chen National Engineering Laboratory for VOCs Pollution Control Technology and Equipment Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution ControlSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510006China National Engineering Laboratory for Mobile Source Emission Control Technology China Automotive Technology&Research Center Co.Ltd.Tianjin 300300China

Palladium-exchanged chabazite(Pd-CHA) zeolites as passive NO_x adsorbers(PNAs) enable efficient purification of nitrogen oxides(NO_x) in cold-start diesel exhausts. Their commercial application, however,is limited by the lack of facile preparation method. Here, high-performance CHA-type Pd-SAPO-34 zeolite was synthesized by a modified solid-state ion exchange(SSIE) method using PdO as Pd precursor,and demonstrated superior PNA performance as compared to Pd-SAPO-34 prepared by conventional wetchemistry strategies. Structural characterization using Raman spectroscopy and X-ray diffraction revealed that the SSIE method avoided water-induced damage to the zeolite framework during Pd loading. Mechanistic investigations on the SSIE process by in situ infrared spectroscopy and X-ray photoelectron spectroscopy disclosed that, while PdO precursor was mainly converted to Pd^(2+) cations coordinated to the zeolite framework by consuming the-OH groups of the zeolite, a portion of PdO could also undergo thermal decomposition to form highly dispersed Pd~0 clusters in the pore channels. This simplified and scalable SSIE method paves a new way for the cost-effective synthesis of defect-free high-performance Pd-SAPO-34 zeolites as PNA catalysts.

关键词： Pd-SAPO-34 Passive NO_x adsorber Pd loading Solid-state ion exchange Pd transformation

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Root nodule-assisted activation for the preparation of micropore-graded porous carbon for VOC adsorption

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Journal of Environmental Sciences 2025年

作者： Longfei Xie Liwen Lu Shiyi Wang Xiaojing Sun Yujing Ji Yuqing Chen Weixiao Peng Miao Yu Haomin Huang Daiqi Ye School of Environment and Energy South China University of Technology Guangzhou 510006 China National Engineering Laboratory for VOCs Pollution Control Technology and Equipment Guangzhou 510006 China Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control (SCUT) Guangzhou 510006 China Guangdong Provincial Engineering and Technology Research Centre for Environmental Risk Prevention and Emergency Disposal South China University of Technology Guangzhou 510006 China

In order to address the evolving emission characteristics of oxygenated volatile organic compounds (Ovocs), it is essential to develop adsorbent materials specifically designed for the efficient adsorption of Ovocs with large kinetic diameters. In this study, we used co-pyrolysis to prepare a series of graded porous carbon materials with well-developed micropores by adjusting the doping ratios of root nodules and pretreated cellulose. The material with root nodule to cellulose mass ratio of 1:1 (TCC-RN-1) exhibited the highest saturated adsorption capacity for butyl acetate (834 mg/g). This can be attributed to enhanced pore size distribution from nodule doping, which facilitates the development of a micropore-graded structure. Additionally, the nodules acted as auxiliary activating agents that enhanced the KOH micropore regulation effect during the activation stage, resulting in the highest micropore volume (0.863 cm³/g). The doping of root nodules facilitated the formation of additional defects on the surface of the porous carbon material, leading to a more disordered arrangement that improved pollutant adsorption. Furthermore, TCC-RN-1 demonstrated good thermal stability in an air atmosphere, maintaining a butyl acetate adsorption capacity exceeding 95 % after five adsorption-desorption cycles. This indicates its favorable potential for industrial applications.

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