Acta Biomaterialia
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2023
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IF 9.7
Chenyi Huang,Jia Tang,Yuanqi Liu,Ting Chen,Junyang Qi,Shengjie Sun,Huisong Hao,Weiwei Zeng,Jing Zhao,Meiying Wu
Nitric oxide (NO) is a crucial gaseous medium for tumor growth and progression, but it may also cause mitochondrial disorder and DNA damage by drastically increasing its concentration in tumor. Due to its challenging administration and unpredictable release, NO based gas therapy is difficult to eliminate malignant tumor at low safe doses. To address these issues, herein, we develop a multifunctional nanocatalyst called Cu-doped polypyrrole (CuP) as an intelligent nanoplatform ( [email protected] ) to deliver the NO precursor BNN6 and specifically release NO in tumors. Under the aberrant metabolic environment of tumors, [email protected] catalyzes the conversion of antioxidant GSH into GSSG and excess H 2 O 2 into ·OH through Cu + /Cu 2+ cycle, which results in oxidative damage to tumor cells and the concomitant release of cargo BNN6. More importantly, after laser exposure, nanocatalyst CuP can absorb and convert photons into hyperthermia, which in turn, accelerates the aforesaid catalytic efficiency and pyrolyzes BNN6 into NO. Under the synergistic effect of hyperthermia, oxidative damage, and NO burst, almost complete tumor elimination is achieved in vivo with negligible toxicity to body. Such an ingenious combination of NO prodrug and nanocatalytic medicine provides a new insight into the development of NO based therapeutic strategies. Statement of significance A hyperthermia-responsive NO delivery nanoplatform ( [email protected] ) based on Cu-doped polypyrrole was designed and fabricated, in which CuP catalyzed the conversion of H 2 O 2 and GSH into ·OH and GSSG to induce intratumoral oxidative damage. After laser irradiation, hyperthermia ablation and responsive release of NO further coupled with oxidative damage to eliminate malignant tumors. This versatile nanoplatform provides new insights into the combined application of catalytic medicine and gas therapy.
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高影响因子
Energies
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2019
·Vol. 12
·期 15
·2966
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IF 2.707
Pijian Gong,Xinxue Li
In this study, NaClO2was selected as a denitration oxidant. In order to clarify the mechanism of NaClO2as an oxidation agent for NO removal efficiency, the effects of H+and other factors (NaClO2concentration, temperature, and the other gas) on the NO removal efficiency were investigated. NaClO2showed a promotional ability on NO removal, whose efficiency increased with the increase of NaClO2concentration. One hundred percent removal efficiency of NO could be achieved when the NaClO2concentration was 0.014 mol/L. Furthermore, raising the reaction temperature benefited the removal of NO. The lower the pH, the better the NO removal efficiency. The promoting effect of H+on the NO removal was studied by the Nernst equation, ionic polarization, and the generation of ClO2. Under the optimal conditions, the best removal efficiency of NO was 100%. Based on the experimental results, the reaction mechanism was finally speculated.Keywords:sodium chlorite (NaClO2);wet scrubbing;removal efficiency;NO reaction mechanism
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CATALYSIS COMMUNICATIONS
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2023
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IF 3.7
Jiuhu Zhao,Huiying Li,Yungang Wang,Rongshu Zhu,Senlin Sun,Jingwen Zhang,Chaolin Li,Mei Hong
Mesoporous In/Hβ-X series catalysts were prepared by desilication method with tetrapropylammonium hydroxide (TPAOH) and indium incorporation for selective catalytic reduction of NO with methane (CH 4 -SCR). The post desilication treatment conditions for preparing In/Hβ-X were optimized. Etching time is the most important desilication parameter influencing the resulting CH 4 -SCR performance of the catalyst. The In/Hβ-3 sample which was etched for 3 h presents the highest NO x conversion, 22% higher than In/H-Beta counterparts using commercial microporous beta. Obvious analysis reveals that besides generating mesopores, controlled desilication can modulate the proportion of InO + active sites and surface oxygen species, allowing more active sites to be exposed.
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JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Shaomian Liu,Yongjun Ji,Wenqing Xu,Jianling Zhang,Ruihuan Jiang,Liang Li,Lihua Jia,Ziyi Zhong,Guangwen Xu,Tingyu Zhu,Fabing Su
Developing efficient catalysts for low reaction-temperature catalytic reduction of NO by CO (CO–DeNO x ) is desirable but very challenging. Here, we report that hierarchically interconnected porous (HIP) Mn x Co 3- x O 4 spinels, synthesized by a facile citric acid-assisted sol–gel method, can act as highly efficient catalysts for CO–DeNO x . The obtained Mn 0.3 Co 2.7 O 4 displayed a much-enhanced catalytic performance with 87% NO removal at 100 °C and a wide active-temperature window (100–400 °C). Its superior activity stems from the following reasons: (i) the high-valence of Mn 3+ , Mn 4+ , and Co 3+ species in the Co–O–Mn structure enables the high catalytic activity and the effective redox-cycling of the Co 3+ and Co 2+ adsorption sites; (ii) the HIP structure can significantly enhance gas diffusion. This work offers an avenue to design metal oxide catalysts for CO–DeNO x by effectively controlling the doping metal concentration and oxidation states of the active components.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Li Liu,Ping Ouyang,Yuhan Li,Youyu Duan,Fan Dong,Kangle Lv
Deeply photocatalytic oxidation of nitrogen oxides is still difficult to achieve, mainly limited by few intrinsic active sites and inefficient carrier separation of photocatalysts. Accordingly, we develop a simple room temperature tactic to introduce oxygen vacancies (OVs) into Bi 3 TaO 7 (BTO). Based on solid experimental and DFT theoretical supports, we explore the mechanism of NO removal over OVs decorated BTO (OVs-BTO). OVs can not only alter the distribution of local electrons to result in the formation of a fast charge transfer channel between OVs and the adjacent Ta atoms, which improves the transport rate of photogenerated carriers; but also function as active sites to adsorb small molecules (NO, O 2 and H 2 O), which being activated and positively drive the NO oxidation reaction. In order to investigate a possible reaction path, a combination of in-situ DRIFTS and simulated Gibbs free energy reveals that the intermediate products of OVs-BTO are helpful to promote the deep oxidation of NO to NO 3 - , while pristine BTO is more likely to produce NO 2 intermediate toxic by-products, which greatly hinders the deep photocatalytic oxidation of NO. This work provides insights into the role of OVs in photocatalysts, and also points out a guideline for the mechanism of semiconductor photocatalysts in eliminating gaseous pollutants .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Hongxia Liu,Hui Mei,Shiping Li,Longkai Pan,Zhipeng Jin,Gangqiang Zhu,Laifei Cheng,Litong Zhang
Bismuth titanate (Bi 12 TiO 20 ) with unique sillenite structure has been shown to be an excellent photocatalyst for environmental remediation. However, the narrow light-responsive range and rapid recombination of photoinduced electrons-holes limit the photocatalytic performance of Bi 12 TiO 20 . To overcome the limitations, a practical and feasible way is to fabricate heterojunctions by combining Bi 12 TiO 20 with suitable photocatalysts. Here, using a facile chemical precipitation method, a novel and hierarchical core–shell structure of n-Bi 12 TiO 20 @p-BiOI (BTO@BiOI) heterojunction was rationally designed and synthesized by loading BiOI nanosheets on BTO nanofibers. The constructed BTO@BiOI composites exhibited significant charge transfer ability due to the synergistic effects of the built-in electric field between BTO and BiOI as well as close interfacial contacts. In addition, the narrow bandgap characteristics of the BiOI led to wide light absorption ranges. Therefore, the BTO@BiOI heterojunction exhibited an improved photocatalytic performance under visible light irradiation. The NO removal efficiency of optimal BTO@BiOI was 45.7%, which was significantly higher compared to that of pure BTO (3.6%) or BiOI (23.1%). Moreover, the cycling experiment revealed that BTO@BiOI composite has a good stability and reusability. The possible mechanism of photocatalytic NO oxidation over BTO@BiOI was investigated in detail.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2021
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IF 5.541
Shengxiong Huang,Yifeng Su,Wei Luo,Qian He,Sheng Huang,Nan Zhou,Zhi Zhou
Pyrolysis is a research hotspot for realizing Chinese Herb residue (CHR) treatment and resource utilization, but there is little reported about in-situ no support catalytic pyrolysis of CHR. In this work, kinetics and no support catalytic pyrolysis characteristics of CHR were studied using a thermogravimetric analyzer and a fix-bed reactor system, respectively. Three groups: Ni-Fe, Ni-Cu and Ni-Co add into CHR and three kinetic methods: Coats-Redfern (CR) method, Flynn-Wall-Ozawa (FWO) method and Distributed Activation Energy Model(DAEM)use for calculate the activation energy, then analyses the gas, bio-oil and char of CHR pyrolysis. The results show that, catalysts can reduce the pyrolysis reaction activation energy. In FWO and DAEM model, the reaction activation energy will increase sharply if the conversion over 0.7. Compare with no catalyst group, add catalyst can restrain gas generation but good for oil production and char formation. Meanwhile, the surface of char is smoother than no catalyst. After test the char, we find that, metals of Ni, Fe, Cu and Co almost enrich in char, which may reuse as catalytic. This study may provide a feasible direction for the industrial application of CHR.
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Surfaces and Interfaces
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2021
·
IF 4.837
Fan Wu,Chuan Pu,Minxian Zhang,Bin Liu,Jingling Yang
Solar photocatalysis is a clean and sustainable approach for removing atmospheric NO, but suffers from unsatisfactory removal efficiency. Efficient charge separation and surface reaction are critical factors ensuring the efficiency of solar energy conversion by photocatalysts. To achieve efficient charge steering and an enhanced surface reaction, we synthesized a bicomponent photocatalyst consisting of multivalent Ag species embedded in defect-rich twin-brush ZnO (Ag/TB-ZnO) with strong metal-support interaction (SMSI). The optimum Ag/TB-ZnO with silver loading of 2.0 wt.% achieved NO oxidation efficiency of 71.0% under a GHSV of 1,200,000 mL h −1 g −1 , and NO 3 − selectivity of 94.8%. Outstanding stability of up to 4 h was demonstrated. This superior performance was attributed to the enhanced efficacy of charge separation and surface reaction by the SMSI effect, surface plasmon resonance effect of metallic Ag and the efficient activation of oxygen species through vacancy-rich TB-ZnO.
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Yucheng Ou,Gangqiang Zhu,Fei Rao,Jianzhi Gao,Jun Chang,Xiaotao Xie,Weibin Zhang,Yu Huang,Mirabbos Hojamberdiev
Coral-like TiO2−δ microstructures with high surface area were synthesized by a simple hydrothermal method, followed by thermal treatment in a N2 atmosphere. The introduction of oxygen vacancies (OVs) to TiO2 significantly improved light absorption and inhibited the recombination of photogenerated charge carriers. Then, multiwalled carbon nanotubes (CNTs) and N-doped carbon quantum dots (N-CQDs) were decorated on the surface of coral-like TiO2−δ microstructures. The CNTs could greatly improve the separation and transfer efficiency of photogenerated charge carriers, while the N-CQDs could further extend light absorption to longer wavelengths, including the IR region. According to the results of electron spin resonance (ESR) spectroscopy, the introduction of OVs to TiO2−δ and surface modification with CNTs and N-CQDs promoted the generation of •O2– and •OH active species. The formation of •O2– and •OH active species on the surface of TiO2−δ/CNTs/N-CQDs played an important role in the deep oxidation and selective conversion of NO into nitrate. Density functional theory calculations revealed the adsorption and reaction sites for H2O and O2 separately in space over the surface of TiO2−δ/CNTs/N-CQDs. Namely, the reaction sites of H2O and O2 are on the surface of TiO2−δ and CNTs, respectively. The electron transfer from TiO2−δ to CNTs was further verified through the differential charge density. This study demonstrates a straightforward approach for designing full-spectrum-responsive photocatalysts with high efficiency, stability, and selectivity for NO removal.
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高影响因子
FUEL
·
2020
·
IF 5.578
Yafeng Fu,Hongliang Li,Hao Mei,Zeyu Feng,Ruxia Chen,Jianbo Li,Yongmei Wang,Wenbiao Fu
In coal preparation plants, the tailing coal slime filter cake contains large amounts of super fine particles. It can be hypothesized that the large quantity of organically contaminated water may be purified by a capable filtration process. Meanwhile, the treatment process would be an adsorbent recycling free process, with a roasting process followed in the industry. In this study, methyl blue (MB) was selected as the target organic contaminant, and its removal by filtration was investigated. Meanwhile, the adsorption capacity of MB on Tween-80-modified filter cake was discussed and the spatial structure of the filter was analyzed by micro-CT. With an increasing Tween-80 concentration, the adsorption efficiency of the MB initially increased and reached the maximum adsorption value when the Tween-80 concentration was 60 mg/L, and there was no negative effect on solid-liquid separation. The micro-CT test results indicate that after the modification of Tween-80, the spatial structure of the filter cake was greatly improved, resulting in a relatively stronger adsorption capacity and a higher filtration efficiency. These findings of this study are of great significance for reducing the pollution of water resources and improving the filtration efficiency in the coal washing plant.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Ying Sun,Shuhang Ren,Yucui Hou,Kai Zhang,Qi Zhang,Weize Wu
A series of environmentally benign functional ionic liquids (ILs) based on l-proline as the anion to efficiently absorb low-concentration NO have been investigated in this work. The results indicate that the ILs with an l-proline anion have high absorption capacities for 0.16 vol % NO, reaching a maximum absorption capacity of 0.51 mol of NO per mol of IL at 30 °C and ambient pressure for l-proline choline IL ([Ch][l-Pro]). The absorbed NO could be recovered from [Ch][l-Pro], and the regenerated IL had no significant loss of NO absorption capacity for at least 7 recycles. We verified the mechanism through both experimental and theoretical methods. The results indicate that the absorption of NO in [Ch][l-Pro] mainly resulted from a chemical process—NO and the secondary amine group in the anion form a NONOate with a chemical formula [l-Pro]−–(NO)–NO. We believe that this efficient and reversible absorption of low-concentration NO by the ILs has potential as a new NO capture technique.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2015
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IF 3.368
Xiaole Weng,Xiaoxia Dai,Qingshan Zeng,Yue Liu,Zhongbiao Wu
Heteropoly acids (HPAs) have been effectively utilized in selective catalytic reduction (SCR) of NO to improve the NH 3 absorption capacity and alkaline/alkali metal resistance for SCR catalysts. However, despite the promise on super-acidities, their other properties that would work on SCR process are still lack of exploration. In this study, a 12-tungstaphosphoric acid (H 3 PW 12 O 40 , HPW) was selected to modify a well-reported CeO 2 catalyst. The resulted CeO 2 /HPW catalyst was subsequently utilized for SCR of NO with excess NH 3 , which revealed a significantly promoted performance in SCR reaction. DRIFT analyses showed that the unique NO 2 absorption capacity of HPW could prevent the NO 2 being further oxidized into nitrate species and the abundant Brønsted acid sites could effectively retain the NH 3 , avoiding them being over-oxidized at evaluated temperatures. The presence of NO 2 was demonstrated able to induce a so called “fast SCR” reaction over the CeO 2 /HPW catalyst, which effectively facilitated the SCR reaction. Furthermore, we have also constructed a CeO 2 @HPW catalyst, which showed an enhanced SO 2 poisoning resistance in SCR reaction.
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高影响因子
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