负载型金属氧化物催化剂分解臭氧的研究

用浸渍法制备了活性炭、γ-氧化铝和分子筛负载的MnO2,CuO,Fe2O3催化剂,并考察了它们对臭氧分解的催化性能。结果表明,MnO2催化剂优于CuO,Fe2O3,催化剂,活性炭为载体的催化剂优于γ-氧化铝和分子筛为载体的催化剂。温度对臭氧催化分解影响很大,在90℃时,MnO2／AC催化剂对臭氧的去除率可达80％以上。当存在一定浓度的水蒸气时,湿度越大,催化性能越差。当臭氧初始质量浓度低于50mg／L时,随着臭氧初始浓度的增加,催化性能有一定的下降。     

Efficient degradation of chlorobenzene in a non-thermal plasma catalytic reactor supported on CeO2/HZSM-5 catalysts

Chlorobenzene removal was investigated in a non-thermal plasma reactor using CeO₂/HZSM-5 catalysts. The performance of catalysts was evaluated in terms of removal and energy efficiency. The decomposition products of chlorobenzene were analyzed. The results show that CeO₂/HZSM-5 exhibited a good catalytic activity, which resulted in enhancements of chlorobenzene removal, energy efficiency, and the formation of lower amounts of by-products. With regards to CO₂ selectivity, the presence of catalysts favors the oxidation of by-products, leading to a higher CO₂ selectivity. With respect to ozone, which is considered as an unavoidable by-product in air plasma reactors, a noticeable decrease in its concentration was observed in the presence of catalysts. Furthermore, the stability of the catalyst was investigated by analyzing the evolution of conversion in time. The experiment results indicated that CeO₂/HZSM-5 catalysts have excellent stability: chlorobenzene conversion only decreased from 78% to 60% after 75 hr, which means that the CeO₂/HZSM-5 suffered a slight deactivation. Some organic compounds and chlorinated intermediates were adsorbed or deposited on the catalysts surface as shown by the results of Fourier Transform Infrared (FT-IR) spectroscopy, scanning electron microscope (SEM) and energy dispersive X-ray spectroscopy (EDS) analyses of the catalyst before and after the reaction, revealing the cause of catalyst deactivation.     

g-C3N4/Cu2O/CF电极制备及在微生物燃料电池中的应用

为了提高微生物燃料电池的产电性能,采用电沉积法将石墨态氮化碳(g-C_3N_4)与氧化亚铜(Cu_2O)负载到碳毡(Carbon felt,CF)表面,制得g-C_3N_4/Cu_2O/CF光电极用于构建微生物燃料电池.通过场发射扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)、傅里叶变换红外光谱(FT-IR)、光生电流曲线(I-T)、线性扫描伏安曲线(LSV)对光电阴极进行光电性能测试,并在白光发光二极管(LED)辐照下研究了以Cu_2O/CF、g-C_3N_4/Cu_2O/CF为阴极光催化微生物燃料电池的产电性能.结果表明,g-C_3N_4/Cu_2O/CF电极中g-C_3N_4分布在Cu_2O之间;g-C_3N_4/Cu_2O/CF光电极能提高光利用率,与Cu_2O/CF光电极相比,光电流密度达到2700 mA·m~(-2),增长幅度达到125%;与Cu_2O/CF阴极微生物燃料电池相比,g-C_3N_4/Cu_2O/CF阴极微生物燃料电池具有更优的产电能力,在白光LED辐照下最大功率密度和光电流密度达到110.7 mW·m~(-2)和1102 mA·m~(-2),增长幅度达到16%和27%.     

Toluene decomposition performance and NOx by-product formation during a DBD-catalyst process

Characteristics of toluene decomposition and formation of nitrogen oxide (NO_x) by-products were investigated in a dielectric barrier discharge (DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide (MnOx), iron oxide (FeOx), cobalt oxide (CoOx) and copper oxide (CuO), supported on Al₂O₃/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO₂ selectivity. In addition,NO_xwas suppressedwith the decrease of specific energy density (SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the CuO catalyst showed the best performance in NO_x suppression. The MnOx catalyst exhibited the lowest concentration of O₃ and highest CO₂ selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression.     

Toluene decomposition performance and NOx by-product formation during a DBD-catalyst process

Characteristics of toluene decomposition and formation of nitrogen oxide (NOx) by-products were investigated in a dielectric barrier discharge (DBD) reactor with/without catalyst at room temperature and atmospheric pressure. Four kinds of metal oxides, i.e., manganese oxide (MnOx), iron oxide (FeOx), cobalt oxide (CoOx) and copper oxide (CuO), supported on Al₂O₃/nickel foam, were used as catalysts. It was found that introducing catalysts could improve toluene removal efficiency, promote decomposition of by-product ozone and enhance CO₂ selectivity. In addition, NOx was suppressed with the decrease of specific energy density (SED) and the increase of humidity, gas flow rate and toluene concentration, or catalyst introduction. Among the four kinds of catalysts, the CuO catalyst showed the best performance in NOx suppression. The MnOx catalyst exhibited the lowest concentration of O₃ and highest CO₂ selectivity but the highest concentration of NOx. A possible pathway for NOx production in DBD was discussed. The contributions of oxygen active species and hydroxyl radicals are dominant in NOx suppression.     

氮掺杂生物炭催化臭氧对于布洛芬的降解特性与机制

系统研究了新型氮掺杂生物炭材料(N-C)催化臭氧对于水中布洛芬(IBP)的氧化降解效能及机制,并深入探究了初始pH、臭氧投加量、催化剂投加量、不同阴离子和背景水质条件对IBP降解效率的影响.结果 表明,相较于一些常见的碳基催化剂(g-C3N4、生物炭、颗粒活性炭)及金属催化剂(MnO2、Fe3O4),N-C催化臭氧体系...     

Remarkable promotion effect of trace sulfation on OMS-2 nanorod catalysts for the catalytic combustion of ethanol

OMS-2 nanorod catalysts were synthesized by a hydrothermal redox reaction method using MnSO₄ (OMS-2-SO₄) and Mn(CH₃COO)₂ (OMS-2-AC) as precursors. SO₄^2 −-doped OMS-2-AC catalysts with different SO₄^2 − concentrations were prepared next by adding (NH₄)₂SO₄ solution into OMS-2-AC samples to investigate the effect of the anion SO₄^2 − on the OMS-2-AC catalyst. All catalysts were then tested for the catalytic oxidation of ethanol. The OMS-2-SO₄ catalyst synthesized demonstrated much better activity than OMS-2-AC. The SO₄^2 − doping greatly influenced the activity of the OMS-2-AC catalyst, with a dramatic promotion of activity for suitable concentration of SO₄^2 − (SO₄/catalyst = 0.5% W/W). The samples were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), inductively coupled plasma optical emission spectroscopy (ICP-OES), NH₃-TPD and H₂-TPR techniques. The results showed that the presence of a suitable amount of SO₄^2 − species in the OMS-2-AC catalyst could decrease the Mn–O bond strength and also enhance the lattice oxygen and acid site concentrations, which then effectively promoted the catalytic activity of OMS-2-AC toward ethanol oxidation. Thus it was confirmed that the better catalytic performance of OMS-2-SO₄ compared to OMS-2-AC is due to the presence of some residual SO₄^2 − species in OMS-2-SO₄ samples.     

Metal loaded zeolite adsorbents for hydrogen cyanide removal

Metal(Cu,Co,or Zn) loaded ZSM-5 and Y zeolite adsorbents were prepared for the adsorption of hydrogen cyanide(HCN) toxic gas.The results showed that the HCN breakthrough capacity was enhanced significantly when zeolites were loaded with Cu.The physical and chemical properties of the adsorbents that influence the HCN adsorption capacity were analyzed.The maximal HCN breakthrough capacities were about the same for both zeolites at 2.2 mol of HCN/mol of Cu.The Cu2p XPS spectra showed that the possible species present were Cu2O and CuO.The N1s XPS data and FT-IR spectra indicated that CNwould be formed in the presence of Cu+/Cu2+ and oxygen gas,and the reaction product could be adsorbed onto Cu/ZSM-5 zeolite more easily than HCN.     

Catalytic decomposition of low level ozone with gold nanoparticles supported on activated carbon

Highly dispersed gold nanoparticles were supported on coal-based activated carbon (AC) by a sol immobilization method and were used to investigate their catalytic activity for low-level ozone decomposition at ambient temperature. Nitrogen adsorption-desorption, scanning electron microscope (SEM), and X-ray photoelectron spectroscopy (XPS) were used to characterize the catalysts before and after ozone decomposition. The results showed that the supported gold nanoparticles prepared with microwave heating were much smaller and more uniformly dispersed on the activated carbon than those prepared with traditional conduction heating, exhibiting higher catalytic activity for ozone decomposition. The pH values of gold precursor solution significantly influenced the catalytic activity of supported gold for ozone decomposition, and the best pH value was 8. In the case of space velocity of 120000 h⁻¹, inlet ozone concentration of 50 mg/m³, and relative humidity of 45%, the Au/AC catalyst maintained the ozone removal ratio at 90.7% after 2500 min. After being used for ozone decomposition, the surface carbon of the catalyst was partly oxidized and the oxygen content increased accordingly, while its specific surface area and pore volume only decreased a little. Ozone was mainly catalytically decomposed by the gold nanoparticles supported on the activated carbon.     

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

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 NH₃ 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°C, 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 Cu²⁺ and monomeric Fe³⁺ are revealed as the predominant copper and iron species. At low temperatures, isolated Cu²⁺ species act as primary active sites for SCR reaction, while monomeric Fe³⁺ 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 Cu²⁺ site, as well as the formation of highly oxidizing Fe₂O₃, thus causing deterioration of catalytic performances.