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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Sulfur-doping promoting peroxone reaction over TiO2 for highly effective NO oxidation at low temperature: Experimental and DFT studies

Mingjia Zhang,Fanyu Meng,Shule Zhang,Yiqing Zeng,Qin Zhong

The peroxone reaction between O 3 and H 2 O 2 over TiO 2 exhibits bright prospects for low-temperature flue gas denitration, which effectively overcomes the limitations of traditional peroxone reaction and remains advanced poison resistant ability. In this study, sulfur-doped TiO 2 was successfully adopted to improve the catalytic performance under low consumption of O 3 and H 2 O 2 , making this technology take a pivotal step towards practical application. Compared with TiO 2 /H 2 O 2 /O 3 system (68% NO conversion), the NO conversion could reach up to 85% in S-doped TiO 2 /H 2 O 2 /O 3 system under test condition (GHSV = 1.2 × 10 5 h −1 , H 2 O 2 /NO = 1.2, and O 3 /NO = 0.5). Characterizations and density functional theory calculations revealed that sulfur-doping modified the local structure of the catalyst, which enables a more effective combination between Ti 5c and hydroperoxyl, thus facilitating the reaction. Besides, the introduction of sulfur could increase the adsorption capacity of NO x and enhance the Lewis acidity of the catalyst, thus improving the NO conversion performance. The stability and applicability of the process were systematically tested from the following aspects: varied gas composition, H 2 O 2 consumption, pH value, and SO 2 /CO concentration. Results revealed that the S-doped TiO 2 /H 2 O 2 /O 3 system exhibited good stability and poison resistant ability, the potential for practical applications.

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ACS Applied Bio Materials · 2019 · IF 0

NIR-Triggered Theranostic Bi2S3 Light Transducer for On-Demand NO Release and Synergistic Gas/Photothermal Combination Therapy of Tumors

Yao Huang,Junqing Huang,Mingyang Jiang,Songjun Zeng

Gaseous therapy based on nitric oxide (NO) has emerged as a potential tumor therapy route. However, the development of a NO generator with precisely controlled NO releasing in the target site is still facing enormous challenges. Herein, a typical NO delivery platform by integrating the hollow structured polydopamine (PDA) coated Bi2S3 nanohybrids (denoted as H-Bi2S3@PDA) with a heat-sensitive S-nitrosothiol (RSNO) molecule was explored for near-infrared (NIR) light-responsive on-demand NO-releasing and synergetic gas/photothermal combination therapy of tumors. The designed H-Bi2S3@PDA nanocomposites hold high photothermal conversion efficiency of 46.13% under irradiation of a NIR laser, leading to NIR light-triggered controllable generation of NO gas via breaking the S–NO bonds of the heat-sensitive RSNO molecules. More importantly, synergistic gas/photothermal therapy of the tumor was also achieved, which presented remarkable inhibition growth and ablation of tumors. These findings provide the opportunity to design a NIR light-activated NO generator with a combination of photothermal materials and heat-sensitive molecules for integrative gas/photothermal therapy in deep tumors.

CAS / MDL: 10035-06-0 9003-39-8
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RSC Advances · 2019 ·Vol. 9 ·期 9 ·4682-4692 · IF 3.049

Effect of initial support particle size of MnOx/TiO2 catalysts in the selective catalytic reduction of NO with NH3

Yang Yang,Zhun Hu,Rongli Mi,Dan Li,Xiang Yong,Huie Yang,Kunfeng Liu

A series of manganese-based catalysts supported by 5–10 nm, 10–25 nm, 40 nm and 60 nm anatase TiO2 particles was synthesized via an impregnation method to investigate the effect of the initial support particle size on the selective catalytic reduction (SCR) of NO with NH3. All catalysts were characterized by transmission electron microscopy (TEM), N2 physisorption/desorption, X-ray diffraction (XRD), temperature programmed techniques, X-ray photoelectron spectroscopy (XPS) and in situ diffuse reflectance infrared transform spectroscopy (DRIFTS). TEM results indicated that the particle sizes of the MnOx/TiO2 catalysts were similar after the calcination process, although the initial TiO2 support particle sizes were different. However, the initial TiO2 support particle sizes were found to have a significant influence on the SCR catalytic performance. XPS and NH3-TPD results of the MnOx/TiO2 catalysts illustrated that the surface Mn4+/Mn molar ratio and acid amount could be influenced by the initial TiO2 support particle sizes. The order of surface Mn4+/Mn molar ratio and acid amount over the MnOx/TiO2 catalysts was as follows: MnOx/TiO2(10–25) > MnOx/TiO2(40) > MnOx/TiO2(60) > MnOx/TiO2(5–10), which agreed well with the order of SCR performance. In situ DRIFTS results revealed that the NH3-SCR reactions over MnOx/TiO2 at low temperature occurred via a Langmuir–Hinshelwood mechanism. More importantly, it was found that the bridge and bidentate nitrates were the main active substances for the low-temperature SCR reaction, and bridge nitrate adsorbed on Mn4+ showed superior SCR activity among all the adsorbed NOx species. The variation of the initial TiO2 support particle size over MnOx/TiO2 could change the surface Mn4+/Mn molar ratio, which could influence the adsorption of NOx species, thus bringing about the diversity of the SCR catalytic performance.

CAS / MDL: 13463-67-7
✓ 已验证 产品关联 DOI PubMed 高影响因子
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

Enhancement of NO oxidation activity and SO2 resistance over LaMnO3+δ perovskites catalysts with metal substitution and acid treatment

Fawei Lin,Jiaming Shao,Hairong Tang,Yan Li,Zhihua Wang,Guanyi Chen,Dingkun Yuan,Kefa Cen

NO x control by catalytic oxidation combined with wet absorption has been a promising technology for the flue gas treatment of industrial boiler and furnace. LaMnO 3+δ perovskites were investigated as catalysts for NO oxidation. The comparison between metal substitution of La and Mn cations was researched. The activity results indicated that La site substitution was more favorable for NO oxidation than Mn site substitution. LaCoMnO exhibited the highest activity in NO oxidation with maximum value of 83.74% at 250 °C. That value further increased to 89.96% after acid etching (LaCoMnO-A), and closely, such high value of 89.78% was achieved at 220 °C. The surface area was significantly improved by acid etching, i.e., from 47.0 m 2 /g to 212.0 m 2 /g, Tremendous changes in crystalline structure and morphology were taken place, i.e., perovskites phase disappeared and MnO 2 was detected instead; compact amorphous particle morphology was replaced by multiple layer structure. Even more, Mn 4+ ions and oxygen vacancies accumulated on the surface were improved. Deservedly, the redox property was enhanced enormously, especially at low temperature. Subsequently, SO 2 poisoning tests were conducted at 250 °C under 20 ppm SO 2 . Interestingly, no decrease was observed for LaCoMnO-A within 480-min SO 2 poisoning test, which was totally contrasted with the nearly complete deactivation results of LaCoMnO. In-situ DRIFTS measurements validated nitrate disappeared and replaced by sulfate formation on the catalyst surface. Merely, under low-concentration SO 2 atmosphere, the monodentate nitrate and bidentate nitrate were destroyed, while the free nitrates exhibited higher resistance. Overall, the acid etching improved the catalyst resistance to SO 2 , which may have the potential to apply in the flue gas treatment of low-sulfur and sulfur-free fuel fired boiler and furnace.

CAS / MDL: 10277-43-7
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CHEMOSPHERE · 2019 · IF 5.108

NO oxidation over Fe-based catalysts supported on montmorillonite K10, γ-alumina and ZSM-5 with gas-phase H2O2

Rongji Cui,Suxia Ma,Jie Wang,Shujun Sun

The catalytic gas-phase H 2 O 2 oxidation of NO was achieved over Fe-based catalysts supported on montmorillonite K10, γ-alumina and ZSM-5. ESR tests illustrate that the three catalysts can catalyze decomposition of H 2 O 2 yielding highly reactive hydroxyl radicals , of which Fe/K10 has the fastest rate, followed by Fe/γ-alumina. Fe 3+ in Fe/K10 and Fe/γ-alumina show lower density of electron cloud due to a strong interaction between Fe 3+ and the support, which benefits the electron transfer from the H 2 O 2 to Fe 3+ , thus favoring the production of hydroxyl radicals. Fe species exist on the surface of Fe/K10 mainly in the form of Fe 2 O 3 , whereas Fe species of Fe/γ-alumina and Fe/ZSM-5 exist mainly in the form of Fe 3 O 4 , and it is found that Fe 2 O 3 is more active than Fe 3 O 4 in catalytic gas-phase H 2 O 2 oxidation of NO. Interestingly, Fe/ZSM-5 has the lowest efficiency in generating hydroxyl radicals, its NO removal efficiency is 90%, which is much higher than 47.5% for Fe/γ-alumina and 62.3% for Fe/K10. In-situ IR results suggested that Fe/ZSM-5 are dual functional in oxidation of NO, that is, whether both Fe ion sites and Brønsted acid sites collectively provide the catalytic functionality. In the meantime, a possible reaction mechanism on catalytic gas-phase H 2 O 2 oxidation of NO over Brønsted acid sites is proposed.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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RSC Advances · 2020 ·Vol. 10 ·期 3 ·1757-1768 · IF 3.119

A direct Z-scheme Bi2WO6/NH2-UiO-66 nanocomposite as an efficient visible-light-driven photocatalyst for NO removal

Yiqiu Liu,Yi Zhou,Qijun Tang,Qian Li,Si Chen,Zhuxing Sun,Haiqiang Wang

To explore an efficient photocatalyst for NO pollution, a direct Z-scheme photocatalytic system is successfully fabricated by coupling Bi2WO6 with NH2-UiO-66 via a simple hydrothermal synthesis technique. The Z-scheme system promotes the NO photocatalytic oxidation activity with an optimum NO removal rate of 79%, which is 2.7 and 1.2 times that obtained by using only pristine Bi2WO6 and NH2-UiO-66, respectively. Simultaneously, superior selectivity for converting NO to NO3−/NO2− is observed. The enhanced photocatalytic performance of the Bi2WO6/NH2-UiO-66 hybrids is attributed to the following two aspects: (i) large specific area of NH2-UiO-66, which exposes more active sites and is beneficial to the adsorption and activation of NO; (ii) outstanding Z-scheme structure constructed between BiWO6 and NH2-UiO-66, which can improve the efficiency of the separation of electron–hole pairs and preserves the strong oxidation ability of hybrids. ESR analysis shows that ·O2− and ·OH contribute to NO removal. A possible photocatalytic mechanism of NO oxidation on the direct Z-scheme photocatalyst (BWO/2NU) under visible light irradiation is proposed. This work displays the BWO/2NU hybrid's potential for treating low-concentration air pollutants, and the proposed Z-scheme photocatalyst design and promotion mechanism may inspire more rational synthesis of highly efficient photocatalysts for NO removal.

CAS / MDL: 10035-06-0 10213-10-2
✓ 已验证 产品关联 DOI PubMed 高影响因子
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ENERGY & FUELS · 2020 · IF 3.421

Novel Method Using Na2S2O8 as an Oxidant to Simultaneously Absorb SO2 and NO from Marine Diesel Engine Exhaust Gases

Hongyuan Xi,Song Zhou,Zhao Zhang

Nitric oxide and sulfur dioxide from the exhaust gases of marine diesel engines are harmful for the environment and human health. Environmentally friendly sodium persulfate, which satisfies the requirements of ships and navigation, was used as the main absorbent for the simultaneous removal of SO2 and NO in a self-designed bubble column reactor with an industrial gas distributor in this work. The focus of this work was the absorption of the insoluble NO. The influences of various parameters including the reaction temperature, Na2S2O8 concentration, NO concentration, pH value of the solution, and presence of coexisting gases on NO absorption were comprehensively and systematically studied according to the different working conditions of marine diesel engines. Furthermore, experiments for simultaneously removing SO2 and NO were conducted. Different from the previous studies, the new experimental results showed that the increase of NO concentration and the pH value of 12 were not conducive to the NO absorption; the highest removal efficiency of NO was at pH of 9; the existence of sulfur dioxide weakened the absorption of nitric oxide; the final products of the simultaneous absorption were sulfate and nitrate according to the product detection results. However, the SO2 and NO in simulated exhaust gases (900 ppm SO2, 1000 ppm NO, 15% O2 and 5% CO2) from marine diesel engines were completely absorbed under nonoptimal conditions (at 70 °C and in a 0.15 mol/L sodium persulfate solution), which indicated that sodium persulfate is promising for use in wet emission control technologies for marine diesel engines.

CAS / MDL: 7775-27-1
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APPLIED SURFACE SCIENCE · 2018 · IF 4.439

CeOP material supported CeO2 catalysts: A novel catalyst for selective catalytic reduction of NO with NH3 at low temperature

Weiyuan Yao,Xiaoqiang Wang,Yue Liu,Zhongbiao Wu

In this paper, Ce O P material (mainly consisted of CePO 4 ) and TiO 2 supported CeO 2 catalysts were prepared by wet impregnation route for the selective catalytic reduction (SCR) of NO with NH 3 . The SCR activity results had revealed that CeO 2 /Ce O P-0.4 catalyst yielded over than 90% NO conversion within the temperature range of 200–300 °C, whereas the deNO x efficiency of CeO 2 /TiO 2 -0.4 catalyst was less than 30% at 200 °C. After a series of characterization tests, it was found that CeO 2 /Ce O P catalysts were of better dispersion of active phase than CeO 2 /TiO 2 owing to the strong interactions between CeO 2 and surficial Ce O species on Ce O P material. Thus, more active oxygen species could participate in the SCR reaction at low temperature. Furthermore, compared to CeO 2 /TiO 2 sample, the surface acidity was greatly enhanced for CeO 2 /Ce O P catalysts by the introduction of the acidic support, benefiting the adsorption of NH 3 . Both of which were attributed to the main reasons of the promoted SCR performance over CeO 2 /Ce O P catalysts. Moreover, the NO x ad-species on CeO 2 /TiO 2 sample were very stable and could hardly react with adsorbed NH 3 , impeding L-H reaction pathway at low temperature.

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Advanced Healthcare Materials · 2018 ·Vol. 7 ·期 24 ·1801094 · IF 5.609

Enhancing the Accumulation of Polymer Micelles by Selectively Dilating Tumor Blood Vessels with NO for Highly Effective Cancer Treatment

Guoqing Wei,Yi Wang,Xuehui Huang,Guang Yang,Jingya Zhao,Shaobing Zhou

The accumulation of nanoparticles in tumors by the enhanced permeability and retention (EPR) effect is effective and well known. However, how to maximize accumulation is still a bottleneck in the development of nanomedicine. Herein, a tumor vascular-targeted hybrid polymeric micelle, which has a great capacity to selectively augment the EPR effect of nanoparticles by dilating tumor blood vessels via the activity of nitric oxide (NO), is presented. Under neutral conditions, the micelle is stable, with a long blood circulation half-life due to the carboxylated poly(ethylene glycol) (PEG) layer; in mildly acidic tumor tissues, the micelle can selectively target the tumor blood vessels by the exposed cyclic Arg-Gly-Asp peptide (cRGD) peptides, which is realized with a pH-dependent hydrolysis of the monomethoxy PEG layer. Simultaneously, exposed copper ions catalyze the decomposition of endogenous NO donors, which generates NO in situ, leading to vasodilation and increased tumor vascular permeability. As a result, the accumulation of nanoparticles is significantly enhanced, and a high accumulation of doxorubicin in tumors is achieved at 48 h after injection. This high dose of therapeutic agent produces a large inhibition of tumor growth (94%) in cancer treatment, and shows no general toxicity, with 100% of the mice surviving the treatment regimen.

CAS / MDL: 129-00-0
✓ 已验证 产品关联 DOI PubMed 高影响因子
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ENERGY & FUELS · 2019 · IF 3.021

Simultaneous Removal of NO and SO2 from Exhaust Gas by Cyclic Scrubbing and Online Supplementing pH-Buffered NaClO2 Solution

Zhitao Han,Tian Lan,Zhiwei Han,Shaolong Yang,Jingming Dong,Deping Sun,Zhijun Yan,Xinxiang Pan,Liguo Song

Experiments were conducted to simultaneously remove NO and SO2 from simulated exhaust gas by cyclic scrubbing and online supplementing pH-buffered NaClO2 solutions in a bench-scale reactor. The effects of key operating parameters on pollutant removal performance had been investigated. The results suggested that an extremely high oxidant utilization rate could be obtained when the oxidant supplementing molar rate approached the oxidant consumption molar rate. Though co-existing SO2 in flue gas would consume a certain amount of the oxidant during the absorption process, the intermediate products of SO32– ions generated from SO2 hydrolysis might be in favor of NO2 absorption to some extent. The introduction of ethanol in scrubbing solution could enhance NOx removal performance largely, which was possibly because of its inhibition effect on SO32– oxidation. The reaction mechanism and reaction products in scrubbing solutions were also discussed roughly through theoretical calculations and ion chromatography analysis.

CAS / MDL: 7758-19-2
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2018 · IF 11.698

Highly efficient (BiO)2CO3-BiO2-x-graphene photocatalysts: Z-Scheme photocatalytic mechanism for their enhanced photocatalytic removal of NO

Yuefa Jia,Shiping Li,Jianzhi Gao,Gangqiang Zhu,Fuchun Zhang,Xianjin Shi,Yu Huang,Chunli Liu

NO removal is one of the most important issues in dealing with air pollution. In this report, Z-scheme (BiO) 2 CO 3 -BiO 2-x -graphene (BOC-BiO 2-x -GR) composite photocatalyst was designed for NO removal under simulated solar light irradiation. Characterizations of physical properties of the ternary composites revealed extended light absorption and high efficient electron-hole separation. Through the optimization of the BiO 2-x content, we observed that the BOC-BiO 2-x (35wt%)-GR composite exhibited superior photocatalytic activities in NO removal as compared to pure BOC, BiO 2-x , and BOC-BiO 2-x binary composites. Detailed microstructural observation showed that the BOC-BiO 2-x heterojunction was formed between BOC (013) and BiO 2-x (111) planes. The density of state (DOS) calculation revealed that due to the different hybridization conditions in the energy bands of BOC and BiO 2-x , the Z-scheme charge transfer should be dominant at the heterojunction interface. The density functional theory (DFT) computation on the Fermi level results confirmed that energy band structure between BOC and BiO 2-x is more in favor of the transfer of photo-generated electrons from CB of BOC to the VB of BiO 2-x , which can be further enhanced by highly conductive GR sheets. The electron spin resonance (ESR) experiments results show that O 2 − and HO were produced during the photocatalytic process, which further provided evidences that the BOC-BiO 2-x (35wt%)-GR composite works as a Z-scheme photocatalyst. This work indicates that Bi-based nanomaterials can be employed as a stable and high efficient solar light active photocatalyst for NO removal in air pollution control.

CAS / MDL: 7782-42-5 99614-02-5
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2013 · IF 2.145

Effect of preparation methods on the performance of CeO2/Al2O3 catalysts for selective catalytic reduction of NO with NH3

Rui-tang Guo,Yue Zhou,Wei-guo Pan,Jie-nan Hong,Wen-long Zhen,Qiang Jin,Cheng-gang Ding,Shi-yi Guo

CeO 2 /Al 2 O 3 catalysts prepared by three methods were investigated for selective reduction of NO with NH 3 . It was found that the catalyst prepared by the single step sol–gel method had the best SCR activity and SO 2 resistance performance. From the results of BET, XRD, TPD and TPR, it can be concluded that large surface area, strong interaction, highly dispersed nano-crystalline ceria , high NH 3 adsorption capacity and good redox ability might be the main reasons for the excellent performance of CeO 2 /Al 2 O 3 catalyst prepared by the single step sol–gel method.

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