JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Youzhou He,Yuwei Tan,Mengyu Song,Qingli Tu,Min Fu,Liangjun Long,Jie Wu,Mengmeng Xu,Xingyan Liu
Photocatalysis technology has been widely adopted to abate typical air pollutants. Nevertheless, developing photocatalysts aimed at improving photocatalytic efficiency is a challenge. Herein, the linker-defect NH 2 -MIL-125(Ti) photocatalyst was synthesized through a convenient one-step heating-stirring method (just adjusting multiple temperatures) to firstly realize efficient photocatalytic performances of NO removal and hydrogen evolution . The optimal sample (named 65-NMIL) with a linker-defect content of 32.08% exhibited a NO removal ratio of 65.49%, which was 37.57% higher than that of pristine NH 2 -MIL-125(Ti), and displayed better H 2 -production activity. Through ESR, it was confirmed that 65-NMIL can generate more •O 2 - and •OH under visible light, and the radical trapping experiment further proved that •O 2 - played a more important role in photocatalytic activity. Moreover, the photocatalytic NO oxidation process was also monitored by in situ DRIFTS , it was found that the defective samples could promote the oxidation of NO and intermediates to the final product (NO 3 - ). On the basis of the above-mentioned photocatalytic experimental results and characterization, a possible mechanism or pathway was proposed and illustrated. This work can provide a new strategy for the subsequent defect engineering for photocatalytic MOFs materials to further solve environmental and energy crises.
研究领域:
材料科学
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光催化
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环境修复
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能量转换
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纳米技术
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JOURNAL OF MEMBRANE SCIENCE
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2026
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IF 8.8
Xiangsen Xu,Qin Huang,Yajing Wu,Yiqing Zeng,Feng Zhang,Zhaoxiang Zhong,Weihong Xing
For catalytic membranes, the loading of catalysts provides the membrane substrate with novel catalytic functionality, while simultaneously inducing membrane surface reconstruction. However, the effect of such surface reconstruction on performance remains unclear. Herein, VCeTi/SiC catalytic membranes with distinct surface structures were fabricated by three distinct preparation routes. Their NH 3 -SCR activity, gas permeance, and separation performance were systematically evaluated. For both VCeTi/SiC-A and VCeTi/SiC–B, the multi-step impregnation and catalyst blockage led to significantly reduced pore sizes (7.6 μm and 5.4 μm) and poor pore size distributions. In contrast, the VCeTi/SiC–C catalytic membrane prepared by single-step solution impregnation method exhibited an optimal catalyst distribution while largely maintaining a concentrated pore size distribution almost identical to the original catalytic membrane. Benefiting from the more uniform gas flow within the carrier owing to its concentrated pore size distribution, it exhibited the widest operating temperature window for NH 3 -SCR with >90% NO conversion from 300 to 450 °C. Meanwhile, VCeTi/SiC–C also displayed the improved pore size (8.0 μm), the highest gas permeance (380 m 3 m −2 h −1 ·kPa −1 ) and the lowest filtration resistance. Furthermore, we discovered "defect-compensating effect" of dust in combined removal experiment, where dust particulates contribute to enhanced denitration performance. This work provides critical insights into the surface design of high-performance catalytic membranes for medium-high temperature gas purification applications.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yangyang Guo,Yang Zheng,Yue Peng,Tao Yue,Tingyu Zhu
Simultaneous removal of NO x and CO from steel sintering has attracted great attention because it is difficult to balance the catalyst reducibility and surface acidity merely using metal oxides or zeolite catalysts. In this study, a mixed CuMn-HZSM-5 catalyst was prepared via an impregnation method. The optimized sample exhibited excellent performance with 90% NO conversion and 100% CO conversion at 175 °C. The activity window of the catalyst was coincident with the actual demand of sintering flue gas control at 150-250℃. The active component CuMn suppressed the excessive Lewis acid sites on the zeolite support for NH 3 adsorption, while the reducibility of the catalyst also decreased compared with that of pure CuMn metal oxides . This synergistic effect was beneficial for the reduction of NH 3 nonselective oxidation with O 2 . In addition, both the DFT and DRIFTS results revealed that NO conversion was improved by CO introduction at low temperature, since NO could adsorb on the CO-preadsorbed sites for the reduction to N 2 via the O atoms of Mn 3c sites, i.e., adsorbed CO could also serve as a reductant to reduce NO to N 2 , which provides another reaction pathway in SCR reactions. Moreover, the NO 2 − and N 2 O 2 − species were observed in the spectra as key intermediates to oxidize CO to CO 2 , which are also the promoters for CO control.
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International Journal of Nanomedicine
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2023
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IF 8
Yan Xu,Jiwei Liu,Zhangya Liu,Guoguang Chen,Xueming Li,Hao Ren
Introduction Limited by tumor vascular barriers, restricted intratumoural T cell infiltration and nanoparticles accumulation remain major bottlenecks for anticancer therapy. Platelets are now known to maintain tumor vascular integrity. Therefore, inhibition of tumor-associated platelets may be an effective method to increase T cell infiltration and drug accumulation at tumor sites. Herein, we designed an ultrasound-responsive nitric oxide (NO) release nanosystem, SNO-HSA-PTX, which can release NO in response to ultrasound (US) irradiation, thereby inhibiting platelet function and opening the tumor vascular barrier, promoting drug accumulation and T cell infiltration.Methods We evaluated the ability of SNO-HSA-PTX to release NO in response to US irradiation. We also tested the effect of SNO-HSA-PTX on platelet function. Plenty of studies including cytotoxicity, pharmacokinetics study, biodistribution, blood perfusion, T cell infiltration, in vivo antitumor efficacy and safety assessment were conducted to investigate the antitumor effect of SNO-HSA-PTX.Results SNO-HSA-PTX with US irradiation inhibited tumor-associated platelets activation and induced openings in the tumor vascular barriers, which promoted the accumulation of SNO-HSA-PTX nanoparticles to the tumor sites. Meanwhile, the damaged vascular barriers allowed oxygen-carrying hemoglobin to infiltrate tumor regions, alleviating hypoxia of the tumor microenvironment. In addition, the intratumoral T cell infiltration was augmented, together with chemotherapy and NO therapy, which greatly inhibited tumor growth.Discussion Our research designed a simple strategy to open the vascular barrier by inhibiting the tumor-associated platelets, which provide new ideas for anti-tumor treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Wenli Liu,Chang Li,Jiaming Mao,Liming Hu,Meng Li,Yanbin Yun,Changyu Lu
Photocatalytic membranes were prepared by hydrothermal method using in situ growth of silica-doped titanium dioxide nanorods with different molar ratios on the surface of hollow ceramic membranes. The removal of nitrogen oxides from high humidity flue gas at ppm level and the recovery of flue gas water vapor were investigated for the first time. The optimized 0.2Si-TiO 2 photocatalytic membrane achieved complete conversion of 50 ppm NO carrying saturated water vapor in only 11 min under UV light source irradiation, and the generation of toxic intermediate product NO 2 was significantly reduced to 4.2 ppm. Further studies have shown that the presence of water vapor can facilitate the conversion of the toxic intermediate NO 2 to nitrate. Moreover, the water vapor recovery flux was 4.18 kg·m −2 ·h −1 , and the water vapor recovery efficiency reached 7.04%. The main water vapor recovery method was membrane condensation. Mechanistic analysis showed that hydroxyl radicals and superoxide radicals are the main components of photocatalytic oxidation, and this work provides a reference for enhancing the photocatalytic conversion of NO and suppressing the emission of toxic intermediates NO 2 in the process.
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ACS Nano
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2023
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IF 17.1
Zhanlin Zhang,Hui Yan,Wenxiong Cao,Shuang Xie,Pan Ran,Kun Wei,Xiaohong Li
Cancer phototherapy indicates advantages in ease of manipulation, negligible drug resistance, and spatiotemporal control but is confronted with challenges in tumor cell accessibility and intermittent light excitation. Herein, we propose a strategy with persistent luminescence (PL)-excited photothermal therapy (PTT), concurrent thermophoresis-propelled motion, and PL-triggered NO release, where PL emission is chargeable by ultrasonication for readily applicable to deep tumors. Mechanoluminescent (ML) nanodots of SrAl2O4:Eu2+ (SAOE) and PL nanodots of ZnGa2O4:Cr3+ (ZGC) were deposited on mesoporous silicates to obtain mSZ nanoparticles (NPs), followed by partially coating with polydopamine (PDA) caps and loading NO donors to prepare Janus mSZ@PDA-NO NPs. The ML emission bands of SAOE nanodots overlap with the excitation band of ZGC, and the persistent near-infrared (NIR) emission could be repeatedly activated by ultrasonication. The PL emission acts as an internal NIR source to produce a thermophoretic force and NO gas propellers to drive the motion of Janus NPs. Compared with the commonly used intermittent NIR illumination at both 660 and 808 nm, the persistent motion of ultrasound-activated NPs enhances cellular uptake and long-lasting PTT and intracellular NO levels to combat tumor cells without the use of any chemotherapeutic drugs. The ultrasound-activated persistent motion promotes intratumoral accumulation and tumor distribution of PTT/NO therapeutics and exhibits significantly higher tumor growth inhibition, longer animal survival, and larger intratumoral NO levels than those who experience external NIR illumination. Thus, this study demonstrates a strategy to activate PL emissions and construct PL-excited nanomotors for phototherapy in deep tissues.
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ENERGY & FUELS
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2022
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IF 4.654
Wei Zhang,Jie Zhao,Ahmed A. Allam,Yue Xin,Jingqi Lin,Ting Gao,Jamaan S. Ajarem,Ximing Li,Chuanyi Wang,Detlef W. Bahnemann
Bi2WO6 is a promising photocatalyst for NOx removal, owing to its wide solar light absorption and specific photoelectric properties. Nevertheless, enhancing its efficiency remains a major concern. Palladium proves to be a good co-catalyst for semiconductor materials, but how the combination of Pd and bismuth tungstate affects the efficiency of NO removal and relevant process is still vague. In this work, nutshell-like bismuth tungstate was synthesized using a hydrothermal method, followed by photo-depositing Pd nanoparticles with different contents. The obtained photocatalysts were characterized by X-ray diffraction, specific surface area analyzer (BET), X-ray photoelectron spectroscopy, and scanning electron microscopy. Among the prepared photocatalysts, Bi2WO6 deposited with 1 wt % Pd shows the best photocatalytic activity with a NO removal efficiency of 58%, which is 2.9 times that of the Bi2WO6 under the same conditions. The enhanced photocatalytic activities were attributed to the comprehensive effects of the high efficiency in separating electrons and holes, improvement in invisible light utilization and BET specific surface areas of Pd–Bi2WO6 nanocomposites. More importantly, it was found that NO2 is the main product over Bi2WO6, whereas the conversion of NO to NO3– (an environmentally friendly product) is dominant over Pd-modified Bi2WO6 due to the enhanced separation of electrons and holes. Active species capture experiments show that photo-generated holes (h+) and •O2– play an important role in NO removal. The present work provides new insights into the role of Pd cocatalysts in NO removal.
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Advanced Healthcare Materials
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2022
·Vol. 11
·期 19
·2201323
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IF 11.092
Shuang Xie,Kun Huang,Jiawen Peng,Yuan Liu,Wenxiong Cao,Dandan Zhang,Xiaohong Li
Diabetic foot ulcer (DFU) treatment is challenged by persistent bacterial infection and hyperglycemia-caused vascular dysplasia. Herein, self-propelled nanomotors are designed to achieve biofilm microenvironment (BME)-activated multistage release of NO for effective sterilization and subsequent angiogenesis promotion. CaO 2 nanoparticles (NPs) are capped with PDA layers, followed by complexation with Fe 2+ and surface grafting of cysteine-NO to obtain Janus Ca@PDA Fe -CNO NPs. In response to low pH in BME, the decomposition of CaO 2 cores generates O 2 from one side of Janus NPs to propel biofilm penetration, and the released H 2 O 2 and Fe 2+ produce •OH through Fenton reaction. The concurrent glutathione-triggered release of NO can be converted into reactive nitrogen species, which exhibit significantly higher bactericidal efficacy than those with only generation of •OH or NO. The slow release of NO for an extended time period promotes endothelial cell proliferation and migration. On Staphylococcus aureus -infected skin wounds of diabetic mice, NP treatment eliminates bacterial infections and significantly elevates blood vessel densities, leading to full wound recovery and regeneration of arranged collagen fibers and skin accessories. Thus, the self-propelling and multistage release of NO provide a feasible strategy to combat biofilm infection without using any antibiotics and accelerate angiogenesis and wound healing for DFU treatment.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
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IF 6.76
Hongyu Zhang,Ling Chen,Baogang Xu,Ping Yang
The strong band-to-band visible light absorption obtained by changing the bandgap of photocatalysts is desirable but challenging for TiO 2 . In this paper, a mechanochemical pre-reaction and subsequent heat-treatment process were used to create TiO 2 /g-C 3 N 4 heterojunctions. Acid-treated H 2 Ti 3 O 7 nanobelts and superior thin g-C 3 N 4 nanosheets (CN) were ground evenly and further heat-treated to grow rhombic TiO 2 in situ on the nanosheets. The heterojunctions exhibited a band gap with the absorption in visible light region. Heterojunction formation effective tunes the surface and electronic structures of the composite, resulting in significant decrease of bandgap. g-C 3 N 4 -based heterojunctions (5TCN) exhibited excellent H 2 generation (4991 μmol/g/h) and NO removal. In contrast, a TiO 2 -based composite (95TCN) revealed efficient photo reduction of Cr(Ⅵ) which was 2 times of that of TiO 2 sample and 22 times of that of CN. The photochemical reaction mechanism of TiO 2 and g-C 3 N 4 -based composites was discussed with the ratio of TiO 2 and g-C 3 N 4 . The excellent performance is ascribed to single crystal rhombic TiO 2 nanoparticles grown in situ on g-C 3 N 4 to form well-developed heterojunctions which accelerate the carrier transfer. These results inspire the electronic structure engineering of photocatalysts to improve visible light absorption and provide a magic strategy for excellent photochemical activities.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Kean Chen,Binxian Chu,Qiuju Qin,Xuemei Ou,Runqi Zhao,Xiaoling Wei,Huan Wu,Bin Li,Lihui Dong
As an ideal substitute for the precious metals in the selective catalytic reduction of NO by CO, transition metal oxides perform very well. Thus, a series of CuO - Co 3 O 4 symbiotic oxide porous nanosheet catalysts are prepared with a CTAB-assisted hydrothermal method. Cu5 with the ratio of Cu and Co is 5 : 10, has the best activity on the premise of maintaining the nanosheet structure. Reduction pretreatment of Cu5 with H 2 is carried out, and the surface will be rapidly oxidized in air. In this period, Cu, CuO and Co 3 O 4 were produced and coexisted on surface. Cu5-re-163 exhibits greatly higher N 2 selectivity but a little inferior NO conversion. Further DFT calculation and characterizations proved that [N] free radicals exist during the reaction. The reaction on Cu5 and Cu-re-163 follow L-H and E-R mechanism respectively. [N] radicals on the latter are much easier to desorb, so that they are easy to combine with each other to form N 2 rather than with NO to generate N 2 O, as the reason why Cu5-re-163 has better selectivity.
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Green Energy & Environment
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2022
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IF 12.781
Yanqin Li,Junqi Tian,Zhisong Liu,Zhongqi Liu,Dong Dong,Fu Wang,Wei Wang,Minmin Liu,Jianming Dan,Yongsheng Li,Feng Yu,Bin Dai,Yunbo Yu
Photo-assisted SCR (PSCR) offers a potential solution for removal of NO at room temperature. MnTiO x as PSCR catalyst exhibits superior performance with NO removal of 100% at the room temperature. Electron paramagnetic resonance (EPR) analysis revealed the presence of numerous oxygen vacancies on MnTiO x . Optical carrier density functional theory (DFT) calculations showed that the three-dimensional orbital hybridization of Mn and Ti is significantly enhanced under light irradiation. The MnTiO x catalyst exhibited excellent electron–hole separation ability, which can adsorbe NH 3 and dissociate to form NH 2 fragments and H atoms. In-situ diffuse reflectance infrared fourier-transform spectroscopy (DRIFTS) indicated that the optical carrier enhanced NH 3 adsorption on MnTiO x , which makes it possess excellent PSCR activity. This work provided an additional strategy to NO removal with PSCR catalysts and showed potential for use in photocatalysis.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Yin Tang,Wen Cui,Songxia Wang,Fan Dong
Though photocatalytic purification of NO has been widely studied, how to avoid secondary pollution during gas-solid reaction is still a challenge, especially in inhibiting the formation of toxic intermediates (NO 2 ) and avoiding the blow away of powdery photocatalyst. Herein, we proposed a one-step solvothermal method to prepare melamine sponge (MS) supported and functionalized g-C 3 N 4 (CN), which simultaneously realizes the inhibition of NO 2 formation and catalyst loss. Sodium hydroxide , which plays a dual role, has been introduced during the preparation of supported photocatalyst. Specifically, sodium atom, as the modifier of performance, could facilitate the randomly distributed charge of pristine CN to be converged, which accelerates the adsorption/activation of reactants for efficient and deep NO oxidation . Hydroxyl group, as the binder between CN and MS, induces the interaction by forming hydrogen bonds , which contributes to the firm immobilization of powdery photocatalyst. The supported sample exhibits outstanding NO removal rate (58.90%) and extremely low NO 2 generation rate (1.41%), and the mass loss rate of photocatalyst before and after reaction is less than 1%. The promotion mechanism of performance also has been elaborated. This work takes environmental risks as a prerequisite to propose a feasible strategy for perfecting the practical application of photocatalytic technology .
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