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

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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Co_(3)O_(4)as an efficient passive NO_(x) adsorber for emission control during cold-start of diesel engines

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Chinese Journal of Chemical engineering 2024年第2期66卷 1-7页

作者： Jinhuang Cai Shijie Hao Yun Zhang Xiaomin Wu Zhenguo Li Huawang Zhao Department of Environmental Science&engineering College of Chemical EngineeringHuaqiao UniversityXiamen 361021China Wuxi Weifu Environmental Catalysts Co. LtdWuxi 214000China national engineering laboratory for mobile source emission control technology China Automotive Technology&Research Center Co.Ltd.Tianjin 300300China

The Co_(3)O_(4)nanoparticles,dominated by a catalytically active(110)lattice plane,were synthesized as a low-temperature NO_(x) adsorbent to control the cold start emissions from vehicles.These nanoparticles boast a substantial quantity of active chemisorbed oxygen and lattice oxygen,which exhibited a NO_(x) uptake capacity commensurate with Pd/SSZ-13 at 100℃.The primary NO_(x) release temperature falls within a temperature range of 200-350℃,making it perfectly suitable for diesel engines.The characterization results demonstrate that chemisorbed oxygen facilitate nitro/nitrites intermediates formation,contributing to the NO_(x) storage at 100℃,while the nitrites begin to decompose within the 150-200℃range.Fortunately,lattice oxygen likely becomes involved in the activation of nitrites into more stable nitrate within this particular temperature range.The concurrent processes of nitrites decomposition and its conversion to nitrates results in a minimal NO_(x) release between the temperatures of 150-200℃.The nitrate formed via lattice oxygen mainly induces the NO_(x) to be released as NO_(2) within a temperature range of 200-350℃,which is advantageous in enhancing the NO_(x) activity of downstream NH_(3)-SCR catalysts,by boosting the fast SCR reaction pathway.Thanks to its low cost,considerable NO_(x) absorption capacity,and optimal release temperature,Co_(3)O_(4)demonstrates potential as an effective material for passive NO_(x) adsorber applications.

关键词： emission control Cold-start Low-temperature adsorption Co_(3)O_(4) Nitrate formation

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Synthesis of chitosan-based grafting magnetic flocculants for flocculation of kaolin suspensions

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Journal of Environmental Sciences 2024年第5期139卷 193-205页

作者： Chuang Liu Xiaoyu Wang Sicong Du Wenyan Liang Beijing Key Lab for source control technology of Water Pollution/engineering Research Center for Water Pollution source control&Eco-remediation/College of Environmental Science and engineering Beijing Forestry UniversityBeijing 100083China

A series of novel chitosan-based magnetic flocculants FS@CTS-P(AM-DMC)was prepared by molecular structure control.The characterization results showed that FS@CTS-P(AM-DMC)had a uniform size of about 21.46 nm,featuring a typical core-shell structure,and the average coating layer thickness of CTS-P(AM-DMC)was about 5.03 nm.FS@CTS-P(AM-DMC)exhibited excellent flocculation performance for kaolin suspension,achieved 92.54% turbidity removal efficiency under dosage of 150 mg/L,pH 7.0,even at high turbidity(2000 NTU)with a removal efficiency of 96.96%.The flocculation mechanism was revealed to be dominated by charge neutralization under acidic and neutral conditions,while adsorption and bridging effects play an important role in alkaline environments.The properties of magnetic aggregates during flocculation,breakage,and regeneration were studied at different pH levels and dosages.In the process of magnetophoretic,magnetic particles collide and adsorb with kaolin particles continuously due to magnetic and electrostatic attraction,transform into magnetic chain clusters,and then further form three-dimensional network magnetic aggregates that can capture free kaolin particles and other chain clusters.Particle image velocimetry confirmed the formation of eddy current of magnetic flocs and experienced three stages:acceleration,stabilization,and deceleration.

关键词： Magnetic flocculation Chitosan Fe_(3)O_(4) Graft copolymerization PIV

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Evolution hydrothermal aging resistance mechanism study of zirconium and manganese doped CeO2 catalysts in soot catalytic combustion based on low Miller indices crystal surface effect

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Journal of Rare Earths 2024年第7期42卷 1272-1281页

作者： Zonglin Li Pan Wang Hong Ni Chengcheng Ao Lidong Zhang Hefeng Zhang Kai Li School of Automotive and Traffic engineering Jiangsu University State Environmental Protection Key laboratory of Vehicle emission control and Simulation Chinese Research Academy of Environmental Science national Synchrotron Radiation laboratory University of Science and Technology of China

The thermogravimetric analysis（TGA） experiments were carried out to reveal the mechanism of Zr and Mn doping on catalytic activity of CeO2catalyst both fresh and after hydrothermal aging,and the lattice morphology and valence changes were characterized by means of Brunauer-Emmett-Teller（BET）method,X-ray diffraction（XRD）,X-ray photoelectron spectroscopy（XPS）,and H2-temperature programmed reduction（H2-TPR）.Density functional theory（DFT） and molecular thermodynamics calculations were applied to investigate the change in catalytic activity,crystal surface energy and crystal morphology caused by hydrothermal aging.The maximum reaction rate temperature of fresh Mn/CeO2（389℃） is similar to that of CeO2（371℃） and lower than that of Zr/CeO2（447℃）,but the catalytic performance of CeO2decreases more severely after hydrothermal aging.The catalyst crystals show different degrees of crystal surface migration after hydrothermal aging,which leads to the reduction of Ce3+/Ce4+ratio and the active sites shift.DFT calculations indicate that the doping of Zr and Mn reduces the surface energy of the low Miller indices surface and increases the oxygen vacancy formation energy,leading to better thermal stability and lower catalytic activity.The Zr and Mn doping also changes the adsorption energy and Gibbs free energy of H2O,which dominates the migration of（1 1 1） to（1 1 0） and（1 0 0） in the vapor environment.The crystal surface migration mechanism of CeO2catalysts doped with Zr and Mn induced by H2O molecules at high temperature obtained in this study can provide a valuable addition to the regeneration of CeO2catalysts in the after-treatment systems of diesel engines.

关键词： CDPF CeO2-based catalyst DFT calculations Rare earth metal oxides Soot

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Low-temperature NH_(3) abatement via selective oxidation over a supported copper catalyst with high Cu^(+) abundance

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Journal of Environmental Sciences 2024年第9期143卷 12-22页

作者： Zhiming Yang Lin Peng Leneng Yang Mingli Fu Daiqi Ye Peirong Chen Guangdong Provincial Key laboratory of Atmospheric Environment and Pollution control National Engineering Laboratory for VOCs Pollution Control Technology and EquipmentSchool of Environment and EnergySouth China University of TechnologyGuangzhou 510006China Guangdong Chengyi Environmental technology Corp. Shaoguan 512158China

Selective catalytic NH_(3)-to-N_(2) oxidation(NH_(3)-SCO)is highly promising for abating NH_(3) emissions slipped from stationary flue gas after-treatment devices.Its practical application,however,is limited by the non-availability of low-cost catalysts with high activity and N_(2) selectivity.Here,using defect-rich nitrogen-doped carbon nanotubes(NCNT-AW)as the support,we developed a highly active and durable copper-based NH_(3)-SCO catalyst with a high abundance of cuprous(Cu^(+))sites.The obtained Cu/NCNT-AW catalyst demonstrated outstanding activity with a T_(50)(i.***.the temperature to reach 50% NH_(3) conversion)of 174℃ in the NH_(3)-SCO reaction,which outperformed not only the Cu catalyst supported on N-free O-functionalized CNTs(OCNTs)or NCNT with less surface defects,but also those most active Cu catalysts in open literature.Reaction kinetics measurements and temperature-programmed surface reactions using NH_(3)as a probe molecule revealed that the NH_(3)-SCO reaction on Cu/NCNT-AW follows an internal selective catalytic reaction(i-SCR)route involving nitric oxide(NO)as a key intermediate.According to mechanistic investigations by X-ray photoelectron spectroscopy,Raman spectroscopy,and X-ray absorption spectroscopy,the superior NH_(3)-SCO performance of Cu/NCNT-AW originated from a synergy of surface defects and N-dopants.Specifically,surface defects promoted the anchoring of Cu O nanoparticles on N-containing sites and,thereby,enabled efficient electron transfer from N to Cu O,increasing significantly the fraction of SCR-active Cu^(+)sites in the catalyst.This study puts forward a new idea for manipulating and utilizing the interplay of defects and N-dopants on carbon surfaces to fabricate Cu^(+)-rich Cu catalysts for efficient abatement of slip NH_(3)emissions via selective oxidation.

关键词： NH_(3)-SCO XANES Localized etching N-doping N_(2) selectivity i-SCR

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Pre-combustion mercury removal with co-production of hydrogen via coal electrolysis

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Journal of Environmental Sciences 2024年第2期136卷 382-389页

作者： Xiang Lyu Runming Tao Tianyu Zhang Chemical and Biomolecular engineering Department Ohio University165 Stocker CenterAthensOH45701USA Electrification and Energy Infrastructures Division Oak Ridge National LaboratoryOak RidgeTN37831USA Beijing Key Lab for source control technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China engineering Research Center for Water Pollution source control&Eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China

Pre-combustion mercury removal via coal electrolysis was performed and investigated on a bench-scale coal electrolytic cell(CEC)systemically,and factorial design was used to determine the effect of different operating conditions(coal particle size,operating temperature,operating cell voltage,and flow rate of slurry)on the percentage of mercury removal,percentage of ash removal,and dry heating value change.The results showed that the operating cell voltage,as well as the interaction between operating cell voltage and coal particle size,are significant factors in the percentage of mercury removal.There is no significant factor in the percentage of ash removal and the dry heating value change,but the coal could be purified while keeping the dry heating value almost constant after electrolysis.A co-product of hydrogen could be produced during coal electrolysis with 50%lower energy consumption compared with water electrolysis.Meanwhile,a mechanism for mercury removal in coal was proposed.The facts indicate that coal electrolysis is a promising method for precombustion mercury removal.

关键词： Pre-combustion mercury removal Coal electrolysis Ash removal Dry heating value Hydrogen production

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Boosting oxygen vacancies by modulating the morphology of Au decorated In_(2)O_(3)with enhanced CO_(2)hydrogenation activity to CH_(3)OH

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Journal of Environmental Sciences 2024年第6期140卷 91-102页

作者： Ruxian Hou Jiewen Xiao Qian Wu Tianyu Zhang Qiang Wang Beijing Key Lab for source control technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China engineering Research Center for Water Pollution source control&Eco-remediation College of Environmental Science and EngineeringBeijing Forestry UniversityBeijing 100083China

CO_(2)hydrogenation to methanol has become one of the most promising ways for CO_(2)utilization,however,the CO_(2)conversion rate and methanol selectivity of this reaction still need to be improved for industrial application.Here we investigated the structure-activity relationship for CO_(2)conversion to methanol of In_(2)O_(3)-based catalysts by modulating morphology and decorating Au.Three different Au/In_(2)O_(3)catalysts were prepared,their activity follow the sequence of Au/In_(2)O_(3)-nanosphere(Au/In_(2)O_(3)-NS)>Au/In_(2)O_(3)-nanoplate(Au/In_(2)O_(3)-NP)>Au/In_(2)O_(3)-hollow microsphere(Au/In_(2)O_(3)-HM).Au/In_(2)O_(3)-NS exhibited the best performance with good CO_(2)conversion of 12.7%,high methanol selectivity of 59.8%,and large space time yield of 0.32 g CH_(3)OH/(hr·gcat)at 300℃.The high performance of Au/In_(2)O_(3)-NS was considered as the presence of Au.It contributes to the creation of more surface oxygen vacancies,which further promoted the CO_(2)adsorption and facilitated CO_(2)activation to form the formate intermediates towards methanol.This work clearly suggests that the activity of In_(2)O_(3)catalyst can be effective enhanced by structure engineering and Au decorating.

关键词： CO_(2)hydrogenation Methanol Au/In_(2)O_(3) Morphology Oxygen vacancies

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Autonomous relative optical navigation based on unified modeling of external systematic errors

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Chinese Journal of Aeronautics 2024年第3期37卷 282-289页

作者： Dayi WANG Bowen SUN Maodeng LI Jiaxing LI Haiyin ZHOU Beijing Institute of Spacecraft System engineering Beijing 100191China College of Sciences National University of Defense TechnologyChangsha 410073China national Key laboratory of Space Intelligent control Beijing Institute of Control EngineeringBeijing 100191China

To solve the problem that external systematic errors of the optical camera cannot be fully estimated due to limited computing resources,a unified dimensionality reduction representation method for the external systematic errors of the optical camera is proposed,and autonomous relative optical navigation is realized.The camera translational and misalignment errors are converted into a three-dimensional rotation error,whose differential model can be established through specific attitude control and appropriate assumption.Then,the rotation error and the relative motion state are jointly estimated in an augmented Kalman filter framework.Compared with the traditional method that estimates the camera translational and misalignment errors,the proposed method reduces the computational complexity in that the estimated state dimension is reduced.Furthermore,as demonstrated by numerical simulation,the estimation accuracy is improved significantly.

关键词： Unified model Systematic errors Optical navigation Observability analysis Calibration

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Autonomous Recommendation of Fault Detection Algorithms for Spacecraft

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IEEE/CAA Journal of Automatica Sinica 2024年第1期11卷 273-275页

作者： Wenbo Li Baoling Ning the national Key laboratory of Science and technology on Space Intelligent control Beijing Institute of Control EngineeringBeijing 100094China the School of Data Science and technology Heilongjiang UniversityHarbin 150001China

Dear Editor, This letter deals with the problem of algorithm recommendation for online fault detection of spacecraft. By transforming the time series data into distributions and introducing a distribution-aware measure, a principal method is designed for quantifying the detectabilities of fault detection algorithms over special datasets.

关键词： fault introducing letter

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Photodegradation of xylene isomers:Kinetics,mechanism,secondary pollutant formation potential and health risk evaluation

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Journal of Environmental Sciences 2024年第2期136卷 658-669页

作者： Xiaoyan Chen Weikun Zhu Sufen Feng Jiangyao Chen Guangdong Key laboratory of Environmental Catalysis and Health Risk control Guangdong Technology Research Center for Photocatalytic Technology Integration and Equipment EngineeringInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key laboratory of Environmental Catalysis and Pollution control Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and HealthSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still unclear.Here,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light sources.Xe lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 min.The xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and carbonyls.Among them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of xylenes.Moreover,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure risk.Therefore,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded xylenes.The findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.

关键词： Isomer aromatics Photodegradation Ozone formation Secondary organic aerosols Health risk

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