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Remarkable N_(2)-selectivity enhancement of NH_(3)-SCR over HPMo modified MnCo-BTC@SiO_(2) catalyst

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Journal of Environmental Sciences 2024年第4期138卷 482-495页

作者： Songjin Ko Xiaolong Tang Fengyu Gao honghong yi Hengheng Liu Ning Luo Department of Environmental Science and Engineering University of Science and Technology BeijingBeijing 100083China Department of Chemistry Pyongyang University of ArchitecturePyongyangDPR of Korea

In this work,the phosphomolybdate(HPMo)modification strategy was applied to improve the N_(2) selectivity of Mn Co-BTC@SiO_(2)catalyst for the selective catalytic reduction of NO_(x),and further,the mechanism of HPMo modification on enhanced catalytic performance was *** Mn Co-BTC@SiO_(2-x) catalysts with different HPMo concentrations,Mn CoBTC@SiO_(2)-0.75 catalyst exhibited not only the highest NH_(3)-SCR performance(95% at 200-300℃)but also the best N_(2)selectivity(exceed 80% at 100-300℃)due to the appropriate redox capacity,greater surface acidity.X-ray photoelectron spectrometer(XPS)and temperature programmed reduction of H_(2)(H_(2)-TPR)results showed that the modification with HPMo reduced the oxidation-reduction performance of the catalyst due to electron transfer from Mo^(5+)to Mn^(4+)/Mn^(3+)and prevent the excessive oxidation of ammonia adsorption ***_(3)temperature-programmed desorption of(NH_(3)-TPD)results showed that the modification with HPMo could significantly improve the surface acidity and NH_(3)adsorption,which enhance the catalytic activity and N_(2)***-situ diffused reflectance infrared Fourier transform spectroscopy(in-situ DRIFTS)revealed that modification with HPMo increased significantly the amount of adsorbed NH_(3)species on the Bronsted acid site and C_(B)/C_(L),it suppressed the production of N_(2)O by inhibiting the production of NH species,the deep dehydrogenation of ammonia adsorption *** study provided a simple design strategy for the catalyst to improve the low-temperature catalytic performance and N_(2)selectivity.

关键词： Metal organic framework(MOF) MnCo-BTC@SiO_(2) NH_(3)-SCR HPMo N_(2)selectivity

Low-temperature NH_(3)-SCR performance of a novel Chlorella@Mn composite denitrification catalyst

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Journal of Environmental Sciences 2024年第3期137卷 271-286页

作者： Hengheng Liu Fengyu Gao Songjin Ko Ning Luo Xiaolong Tang Erhong Duan honghong yi Yuansong Zhou School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing 100083China School of Environmental Science and Engineering University of Science and Technology HebeiHebei 050018China Department of Chemistry Pyongyang University of ArchitecturePyongyangDemocratic People’s Republic of Korea

The synthesis process of conventional Mn-based denitrification catalysts is relatively complex and *** this paper,a resource application of chlorella was proposed,and a Chlorella@Mn composite denitrification catalyst was innovatively synthesized by electrostatic *** Chlorella@Mn composite denitrification catalyst prepared under the optimal conditions(0.54 g/L Mn^(2+)concentration,20 million chlorellas/mL concentration,450℃ calcination temperature)exhibited a well-developed pore structure and large specific surface area(122 m^(2)/g).Compared with MnOx alone,the Chlorella@Mn composite catalyst achieved superior performance,with~100%NH_(3)selective catalytic reduction(NH_(3)-SCR)denitrification activity at 100-225℃.The results of NH_(3)temperature-programmed desorption(NH_(3)-TPD)and H_(2)temperature-programmed reduction(H_(2)-TPR)showed that the catalyst had strong acid sites and good redox *** potential testing showed that the electronegativity of the chlorella cell surface could be used to enrich with Mn^(2+).X-ray photoelectron spectroscopy(XPS)confirmed that Chlorella@Mn had a high content of Mn^(3+)and surface chemisorbed ***-situ diffuse refectance infrared Fourier transform spectroscopy(in-situ DRIFTS)experimental results showed that both Langmuir-Hinshelwood(L-H)and Eley-Rideal(E-R)mechanisms play a role in the denitrification process on the surface of the Chlorella@Mn catalyst,where the main intermediate nitrate species is monodentate *** presence of SO_(2)promoted the generation and strengthening of Bronsted acid sites,but also generated more sulfate species on the surface,thereby reducing the denitrification activity of the Chlorella@Mn *** Chlorella@Mn composite catalyst had the characteristics of short preparation time,simple process and low cost,making it promising for industrial application.

关键词： Chlorella@Mn catalyst NH_(3)-SCR Poisoning resistance Reaction mechanism Infuence of SO_(2)

Morphology and valence state evolution of Cu:Unraveling the impact on nitric oxide electroreduction

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Journal of Energy Chemistry 2024年第4期91卷 276-286页

作者： Ting Sun Fengyu Gao Ya Wang honghong yi Qingjun Yu Shunzheng Zhao Xiaolong Tang School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China

Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas ***,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption and waste gas *** address this,electrocatalytic nitric oxide reduction reaction(NORR)has emerged as a promising strategy to bridge NH3consumption to NH3production,harnessing renewable electricity for a sustainable ***(Cu)stands out as a prominent electrocatalyst for NO reduction,given its exceptional NH3yield and ***,a crucial aspect that remains insufficiently explored is the effects of morphology and valence states of Cu on the NORR *** this investigation,we synthesized CuO nanowires(CuO-NF)and Cu nanocubes(Cu-NF)as cathodes through an in situ growth ***,CuO-NF exhibited an impressive NH3yield of 0.50±0.02 mg cm^(-2)h^(-1)at-0.6 V *** hydrogen electrode(RHE)with faradaic efficiency of29,68%±1,35%,surpassing that of Cu-NF(0.17±0.01 mg cm^(-2)h^(-1),16.18%±1.40%).Throughout the electroreduction process,secondary cubes were generated on the CuO-NF surface,preserving their nanosheet cluster morphology,sustained by an abundant supply of subsurface oxygen(s-O)even after an extended duration of 10 h,until s-O depletion ***,Cu-NF exhibited inadequate s-O content,leading to rapid crystal collapse within the same *** distinctive current-potential relationship,akin to a volcano-type curve,was attributed to distinct NO hydrogenation *** Tafel analysis revealed the exchange current density(i0)and standard heterogeneous rate constant(k0)for CuO-NF,yielding 3.44×10^(-6)A cm^(-2)and 3.77×10^(-6)cm^(-2)s^(-1)when NORR was driven by *** findings revealed the potential of CuO-NF for NO reduction and provided insights into the intricate interplay between crystal morphology,valence states,and electrochemical performance.

关键词： NORR Ammonia Synthesis Copper Morphology Valence States Mechanism

Co-or Ni-modified Sn-MnO_(x) low-dimensional multi-oxides for high-efficient NH_(3)-SCR De-NO_(x):Performance optimization and reaction mechanism

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Journal of Environmental Sciences 2022年第3期34卷 204-218页

作者： Fengyu Gao Chen Yang Xiaolong Tang honghong yi Chengzhi Wang School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants University of Science and Technology BeijingBeijing 100083China

NH_(3)-SCR performances were explored to the relationship between structure morphology and physio-chemical properties over low-dimensional ternary Mn-based catalysts prepared by one-step synthesis *** to its strong oxidation performance,Sn-MnO_(x) was prone to side reactions between NO,NH_(3)and O_(2),resulting in the generation of more NO_(2)and N_(2)O,here most of N_(2)O was driven from the non-selective oxidation of NH_(3),while a small part generated from the side reaction between NH_(3)and NO_(2).Co or Ni doping into Sn-MnO_(x) as solid solution components obviously stronged the electronic interaction for actively mobilization and weakened the oxidation performance for signally reducing the selective tendency of side reactions to N_(2)*** optimal modification resulted in improving the surface area and enhancing the strong interaction between polyvalent cations in Co/Ni-Mn-SnO_(2)to provide more surface adsorbed oxygen,active sites of Mn^(3+) and Mn^(4+),high-content Sn^(4+) and plentiful Lewis-acidity for more active intermediates,which significantly broadened the activity window of Sn-MnOx,improved the N^(2) selectivity by inhibiting N_(2)O formation,and also contributed to an acceptable resistances to water and *** low reaction temperatures,the SCR reactions over three catalysts mainly obeyed the typical Elye-rideal(E-R)routs via the reactions of adsorbed L-NH_(x)(x=3,2,1)and B-NH_(4)^(+) with the gaseous NO to generate N_(2) but also N_(2)O *** for the above basic E-R reactions,as increasing the reaction temperature,the main adsorbed NO_(x)-species were bidentate nitrates that were also active in the Langmuir-Hinshelwood reactions with adsorbed L-NH_(x) species over Co/Ni modified Mn-SnO_(2) catalyst.

关键词： Low-dimensional catalysts One-step synthesis Mn-SnO_(2)nanosheet Ni or Co modification SCR performances Promotional mechanism

Promotional catalytic activity and reaction mechanism of Ag-modified Ce_(0.6)Zr_(0.4)O_(2) catalyst for catalytic oxidation of ammonia

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Journal of Environmental Sciences 2023年第2期124卷 491-504页

作者： Xiaolong Tang Yuanyuan Zhang Yaru Lei Yuanyuan Liu honghong yi Fengyu Gao School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing 100083China

Ce1-xZrxO_(2) composite oxides(molar,x=0-1.0,interval of 0.2)were prepared by a cetyltrimethylammonium bromide-assisted precipitation *** enhancement of silver-species modification and catalytic mechanism of adsorption-transformationdesorption process were investigated over the Ag-impregnated catalysts for lowtemperature selective catalytic oxidation of ammonia(NH_(3)-SCO).The optimal 5 wt.%Ag/Ce_(0.6)Zr_(0.4)O_(2) catalyst presented good NH_(3)-SCO performancewith>90% NH_(3) conversion at temperature(T)≥250°C and 89% N_(2) *** the irregular block shape and underdeveloped specific surface area(∼60m2/g),the naked and Ag-modified Ce_(0.6)Zr_(0.4)O_(2) solid solution still obtained highly dispersed distribution of surface elements analyzed by scanning electron microscope-energy dispersive spectrometer(SEM-EDS)(mapping),N_(2) adsorptiondesorption test and X-ray diffraction(XRD).H2 temperature programmed reduction(H2-TPR)and X-ray photoelectron spectroscopy(XPS)results indicated that Ag-modification enhanced the mobility and activation of oxygen-species leading to a promotion on CeO_(2) reducibility and synergistic Ag0/Ag+and Ce^(4+)/Ce^(3+)redox ***,Ag+/Ag_(2)O clusters could facilitate the formation of surface oxygen vacancies that was beneficial to the adsorption and activation of ***3-temperature programmed desorption(NH_(3)-TPD)showed more adsorption-desorption capacity to ammoniawere provided by physical,weakandmedium-strong acid *** reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments revealed the activation of ammonia might be the control step of NH3-SCO procedure,during which NH3 dehydrogenation derived from NHx-species and also internal selective catalytic reduction(i-SCR)reactions were proposed.

关键词： Ag/Ce_(0.6)Zr_(0.4)O_(2)catalyst Synergistic interaction Catalytic oxidation of ammonia NH3 dehydrogenation Internal selective catalytic reduction

Development of Mn-Si-MEL as a bi-functional adsorption-catalytic oxidation material for VOCs elimination

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Chinese Chemical Letters 2022年第6期33卷 3087-3090页

作者： Qingjun Yu Yongchao Feng Jinghui Wei Xiaolong Tang honghong yi School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China Beijing Key Laboratory of Recycling of Typical Industrial Pollutants Beijing 100083China

Mn-Si-MEL zeolite was developed as a bi-functional adsorption-catalytic oxidation material for volatile organic compounds(VOCs)elimination due to its good hydrophobicity&good organophileproperty brought by the substitution of Mn for Al in zeolite and the superior catalytic oxidation property endowed by the existence of Mn *** Mn-Si-MEL samples were obtained by introducing Mn to MEL crystallization system via different *** was found the incorporated Mn ways have a significant effect on the behavior of Mn being involved in the crystallization of MEL and finally influenced the distribution of Mn in zeolite as well the physicochemical properties of product *** seeding method(MnS2(Seed))is favorable for the good incorporation and uniform distribution of Mn in zeolite while both recrystallization method(Mn-S2(RC))and direct synthesis method(Mn-S2(DH))are favorable for obtaining more reducible Mn species and surface adsorbed oxygen *** Mn amount incorporated into zeolite follows Mn-S2(RC)(1.96 wt%)>Mn-S2(Seed)(1.07 wt%)≈Mn-S2(DH)(0.97 wt%),the adsorption capacity of various samples follows Mn-S2(Seed)(83.3μmol/g)≈Mn-S2(RC)(82.1μmol/g)>Mn-S2(DH)(76.1μmol/g),while the catalytic oxidation ability of three samples follows Mn-S2(RC)≈Mn-S2(DH)>Mn-S2(Seed).Furthermore,Mn-S2(RC)which exhibits both superior adsorption capacity and catalytic oxidation ability shows good hydrophobicity and superior recyclability,demonstrating its great potential to be applied in the VOCs elimination by an enrichment-degradation route.

关键词： Bifunctional Adsorption Catalytic combustion VOCs MEL Mn-Si

Study on mechanism of low-temperature oxidation of n-hexanal catalysed by 2D ultrathin Co_(3)O_(4) nanosheets

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Nano Research 2022年第2期15卷 1660-1671页

作者： Leilei Miao Xiaolong Tang Shunzheng Zhao Xizhou Xie Chengcheng Du Tian Tang honghong yi Department of Environmental Enginnering School of Energy and Environmental EngineeringUniversity of Science and TechnologyBeijingBeijing 100083China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing 100083China

Achieving high catalytic performance with lower possible cost and higher energetic efficiency is critical for catalytic oxidation of volatile organic compounds(VOCs).However,traditional thermocatalysts generally undergo low catalytic activity and fewer active ***,this paper synthesizes nearly all-surface-atomic,ultrathin two-dimensional(2D)Co_(3)O_(4) nanosheets to address these problems through offering a numerous active sites and high electron *** 2D Co_(3)O_(4) nanosheets(1.70 nm)exhibit catalyzation to the total oxidation of n-hexanal at the lower temperature of r90%=202℃,and at the space velocity of 5.0×10^(4) h^(-1).It is over 1.2 and 6 times higher catalytic activity than that of 2D CoO nanosheets(1.71 nm)and bulk Co_(3)O_(4) counterpart,*** absorption spectroscopy analysis shows that the oxygen vacancy defect traps electrons,thereby preventing the recombination with holes,increasing the lifetime of electrons,and making electron-holes reach a nondynamic *** longer the electron lifetime is,the easier the oxygen vacancy defects capture ***,the defects combine with oxygen to form active oxygen *** with the lattice oxygen involved in the reaction of bulk Co_(3)O_(4),the nanosheets change the catalytic reaction path,which effectively reduces the activation energy barrier from 34.07 to 27.15 kJ/*** changed surface disorder,the numerous coordinatively-unsaturated Co atoms and the high ratio of O_(ads)/O_(lat) on the surface of 2D Co_(3)O_(4) nanosheets are responsible for the catalytic performance.

关键词： catalytic reaction n-hexanal oxidation two-dimensional nanosheets oxygen vacancy defect coordinated unsaturated atom

Mesoporous molecular sieve-based materials for catalytic oxidation of VOC: A review

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Journal of Environmental Sciences 2023年第3期125卷 112-134页

作者： Wei Gao Xiaolong Tang honghong yi Shanxue Jiang Qingjun Yu Xizhou Xie Ruijie Zhuang Department of Environmental Science and Engineering School of Energy and Environmental EngineeringUniversity of Science and Technology BeijingBeijing 100083China State Environmental Protection Key Laboratory of Food Chain Pollution Control Beijing Technology and Business UniversityBeijing 100048China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing 100083China

As the main contributor of the formation of particulate matter as well as ozone, volatile organic compounds(VOCs) greatly affect human health and the environmental quality. Catalytic combustion/oxidation has been viewed as an efficient, economically feasible and environmentally friendly way for the elimination of VOCs. Supported metal catalyst is the preferred type of catalysts applied for VOCs catalytic combustion because of the synergy between active components and support as well as its flexibility in the composition. The presence of support not only plays the role of keeping the catalyst with good stability and mechanical strength, but also provides a large specific surface for the good dispersion of active components, which could effectively improve the performance of catalyst as well as decrease the usage of active components, especially the noble metal amount. Mesoporous molecular sieves, owing to their large surface area, unique porous structures, large pore size as well as uniform pore-size distribution, were viewed as superior support for dispersing active components. This review focuses on the recent development of mesoporous molecular sieve supported metal catalysts and their application in catalytic oxidation of VOCs. The effect of active component types, support structure, preparation method, precursors, etc. on the valence state, dispersion as well as the loading of active species were also discussed and summarized. Moreover, the corresponding conversion route of VOCs was also *** review aims to provide some enlightment for designing the supported metal catalysts with superior activity and stability for VOCs removal.

关键词： Volatile organic compound Mesoporous molecular sieves Supported catalyst Catalytic oxidation Reaction mechanism Influencing factors

Novel Mn-Ce bi-oxides loaded on 3D monolithic nickel foam for low-temperature NH_(3)-SCR de-NO_(x):Preparation optimization and reaction mechanism

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Journal of Rare Earths 2022年第2期40卷 268-278,I0003页

作者： Shuquan Ni Xiaolong Tang honghong yi Fengyu Gao Chengzhi Wang yiran Shi Runcao Zhang Wenjuan Zhu School of Energy and Environmental Engineering University of Science and Technology BeijingBeijing 100083China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing 100083China

This study explored the superior citrate method(CM)to synthesize Mn-Ce bi-oxides on 3 D monolithic Ni-foam(NF)catalysts for the selective catalytic reduction of NO by NH_(3)(NH_(3)-SCR).The 17 wt%Mn(7)Ce(3)O_(x)/NF(CM-17)catalyst shows the NO_(x)conversion of 98.7%at 175℃and 90%in the presence of 10 vol%H2 *** is revealed that the combination of surface-active oxygen(formed by high-level oxygen vacancies)and strongly oxidized Mn4+species promots the Fast-SCR reactions,in which Mn4+species play a leading role in NH_(3)-SCR reaction,and the unsaturated Ni atoms and also Ce3+species promote electron exchange and thus improve the redox *** coexistence mechanisms of Fast-SCR reactions and E-R pathways are observed over Mn-CeO_(x)/NF catalyst,which may be promoted by the Br?nsted sites at low *** addition,the heat resistance,stability,3 D monolithic porous structure and excellent physical properties of foam nickel provide a unique growth substrates for catalysts preparation and reaction sites for NO_(x)***,industrial application of Mn-Ce bioxides loaded on 3 D monolithic is proposed to be achieved through reasonable preparation methods.

关键词： NH_(3)-SCR Low temperature Citrate method Fast-SCR 3D monolithic catalysts Oxygen vacancies