Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Ji Liu,Yuan-gu Xia,Meng-fan Liu,Bin Hu,Hong-jin Zhang,Ji-hong Li,Zhen-xi Zhang,Qiang Lu
Nitrogen oxides are the major pollutants in solid fuel/waste combustion processes, which can be reduced by unburned or additive chars. The surface char–NO reaction is significantly influenced by CO 2 , whereas the impact mechanism is far from conclusive. Herein, fixed-bed experiments and computational methods were adopted to elucidate the role of CO 2 on char–NO reaction. Experimentally, CO 2 exhibited an inhibitive impact on NO reduction at 873 K but a promotive influence at 1023 K and 1173 K. According to the detection of outlet CO, characterization of char, and density function theory (DFT) calculations, CO and gasified char derived from char–CO 2 gasification are both responsible for the promotive effect at 1173 K, which offers a clear image of the gasification mechanism conjectured in previous work. More importantly, a CO 2 -mediated oxygen rearrangement (CO 2 -MOR) mechanism has been found and confirmed for the first time, which can well explain the experimental results observed at 873 K and 1023 K. The adsorbed CO 2 can intervene in the oxygen rearrangement on the char surface to alter the NO reduction behaviors. The present study offers a comprehensive insight into the roles of CO 2 in the heterogeneous reduction of NO on char surface.
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PROGRESS IN ORGANIC COATINGS
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2025
·
IF 7.3
Changjiang Pan,Naiquan Yang,Jie Chen,Yan Ji,Linhong Deng,Qingping Xiong
As a versatile biomaterial, polyurethane (PU) finds extensive use in blood-contacting medical devices, including vascular grafts, central venous catheters, hemodialysis catheters, artificial heart valves, and blood oxygenators, etc. However, surface-induced thrombosis and difficulty in surface endothelialization after implantation are potential factors limiting their long-term use. In the present study, a lysozyme nanoparticle biomimetic coating (PTL) was first built on the PU surface based on the phase transition reaction of lysozyme. Subsequently, through sequential amidation reactions, heparin with anticoagulant performances and selenocystamine capable of catalyzing nitric oxide (NO) generation were immobilized onto the PTL surface, yielding a multifunctional nano-biomimetic coating with NO-generation and anticoagulant activities. The coating exhibited outstanding wettability, the ability to inhibit fibrinogen adsorption, and the capacity to catalyze NO generation from NO donors continuously. The as-prepared coating could reduce platelet adhesion, activation, and hemolysis, displaying superior anticoagulant performance. Meanwhile, the coating could promote endothelial cell (EC) proliferation and functional expression (vascular endothelial growth factor (VEGF) and NO) while significantly impeding smooth muscle cell (SMC) adhesion and proliferation, showing a good ability to facilitate endothelialization. Additionally, in the presence of NO donors, the coating could catalyze the NO liberation from donors continuously, further enhancing the blood compatibility and facilitating EC growth selectively. As a consequence, the strategy of this study can simultaneously impart PU with excellent hemocompatibility and rapid endothelialization, providing a new way for constructing anticoagulant and endothelium-promoting nano-biomimetic coatings on PU surfaces.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2025
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IF 4.7
Yinming Fan,Yuanzhen Li,Siqi Jiang,Yanping Zhang,Yinian Zhu,Shengpeng Mo,Lei Liao,Yanan Zhang,Xiaobin Zhou,Zongqiang Zhu
Volatile organic pollutants (VOCs) can serve as an alternative to ammonia for NO reduction, thereby enabling the simultaneous removal of VOCs and NO. In this study, different morphologies of MnO x /CoO x catalysts derived from MOFs were controllably synthesized under various hydrothermal synthesis conditions for the simultaneous removal of 1,2-propanediol and NO. Among the various samples, sample A, characterized by its rod-like structure, demonstrated superior catalytic activity. It achieved simultaneous photothermal coupling for the degradation of 1,2-propanediol and NO under UV irradiation at 240 °C, with conversion rates reaching 52 % and 67 %, respectively. The morphology of the catalysts significantly influences their catalytic performance. The incorporation of Mn increased the structural disorder of the material, thereby reducing the coordination order of Co. This significant change in the coordination environment modulates the intrinsic catalytic activity of the samples, leading to distinct catalytic properties. Furthermore, the catalytic reaction mechanisms were clarified utilizing in-situ DRIFTS combined with calculations based on Density Functional Theory. Sample A, featuring abundant unsaturated cobalt and manganese defects within its distinctive coordination configuration, greatly promoted the conversion of 1,2-propanediol into crucial intermediate species. This study presents a novel approach for the synergistic removal of VOCs and NO x .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Wenjie He,Jiazhen Liao,Lin Jing,Xiao Zhang,Rong Xiao,Peng Chen,Xing'an Dong,Wendong Zhang,Yan Zou,Yuechang Wei
Herein, Br − and Bi 0 co-modified Bi 2 WO 6-x nanosheets were synthesized for efficient photocatalytic NO removal. Plasmonic metallic Bi 0 markedly enhanced visible light absorption, and the Br − -Bi 0 synergistic interaction facilitated efficient separation and migration of photogenerated carriers. Consequently, the optimal catalyst achieved a maximum visible-light-driven NO removal efficiency of 53.1% with near-zero toxic NO 2 accumulation, significantly outperforming pristine Bi 2 WO 6-x (4.6%). Quenching experiments reveal that NO activation and oxidation are dominated by photogenerated e − and •O 2 − radicals, while photogenerated h + drives the subsequent deep oxidation of NO 2 . In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) combined with density functional theory (DFT) calculations confirm the coexistence of direct (NO → NO − → NO 3 − ) and indirect (NO → NO 2 − → NO 3 − ) NO deep oxidation pathways. The Br − -Bi 0 synergy promotes the NO 2 − -to-NO 3 − step, effectively suppressing toxic NO 2 accumulation. This work provides mechanistic insights into the design of advanced photocatalysts for safe and efficient atmospheric pollutant purification.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Yue Li,Junhao Zhou,Xiaoping He,Youzhou He,Jiajia Jing,Xingyan Liu,Siqi Li,Siping Wei
Under the global dual-carbon goal, photocatalysis technology is being employed as a green technology for NO removal and hydrogen production . However, the application of photocatalysts is often limited by the weak response to visible light and the low separation efficiency of photogenerated carriers. In this paper, we designed a simple and efficient photocatalyst Au@NM-125/PdTCPP for NO removal and hydrogen evolution . By adding PdTCPP molecule with excellent light absorption ability combine with MIL-125-NH 2 (Ti), the introduction of PdTCPP expands the absorption range of visible light. On the other hand, the introduction of Au NPs with surface plasmon resonance effect promotes electron transport between PdTCPP and MIL-125-NH 2 (Ti), thus greatly improving the photocatalytic performance. Compared with the NO removal efficiency of the original NM-125 (22.06 %), the NO removal rate of NM-125/PdTCPP was 63.72 %, while the NO removal rate of Au@NM-125/PdTCPP was the highest, reaching 73.23 %. What’s more, Au@NM-125/PdTCPP also demonstrated excellent hydrogen evolution performance (12.659 mmol/g, in 4 h), with a hydrogen evolution effect 2.14 times that of NM-125/PdTCPP (5.911 mmol/g, in 4 h) and 6.85 times that of the initial material NM-125 (1.848 mmol/g, in 4 h). Based on the results of UV-Vis spectroscopy, Mott-Schottky and XPS spectrum, we proposed a possible photocatalytic mechanism, the suitable band gap value of MIL-125-NH 2 (Ti) and PdTCPP makes them form a Z-scheme heterojunction , where electrons flow from PdTCPP to MIL-125-NH 2 (Ti), and Au NPs acts as an electron bridge to promote more electron transfer, thus improving the photocatalytic performance. It is a practicable strategy to achieve excellent photocatalytic performance by combining metalloporphyrin molecules as semiconductors directly with MOFs to form heterojunctions and adding Au NPs as electronic bridges, which is also valuable for environmental remediation and energy production.
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Journal of Physical Chemistry Letters
·
2023
·
IF 5.7
Ying Jiang,Guozhong Lu,Shinuo Kang,Fushan Geng,Bingwen Hu
All-solid-state batteries with ultrathin lithium metal, close to the anode-free solid-state batteries, could achieve high energy density. However, it is not trivial to plate an ultrathin lithium metal layer on a Cu current collector (Cu-CC). In situ electron paramagnetic resonance (EPR) imaging showed that the pre-plating on Cu-CC in a Li–In|Li6PS5Cl|Cu cell without pressure holding produced a lithium metal layer with a small area. However, when a Li–In|Li6PS5Cl|Cu cell was held under a considerable pressure, this cell would produce a lithium metal layer with a large area. The Cu-CC with the ultrathin lithium metal layer of a small surface could be extracted and then assembled with LiNiO2 and Li6PS5Cl to achieve better electrochemical performance compared to that of a large surface, because a small area of the lithium metal layer would lead to fewer side reactions and less consumption of lithium ions. This work suggests the importance of the control of the lithium plating and the observation of lithium plating by in situ EPR imaging.
研究领域:
材料科学
·
电化学
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储能技术
·
固态电池技术
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Xiaosheng Huang,Fang Dong,Guodong Zhang,Zhicheng Tang
In heterogeneous catalysis, the migration and aggregation of active nanoparticles has always been a challenging problem in catalyst design. Two types of confined catalysts, including the pore confined Pore-CeW/OMT and framework confined FW-CeW/OMT were successfully designed for NH 3 -SCR process in this work. Experimental results revealed that the framework confined structure could effectively prevent the migration and aggregation of highly dispersed nanoparticles on catalyst. Benefiting from the structural advantages of ordered mesopores TiO 2 (OMT), large specific surface area as well as abundant active sites could be supplied for catalytic reaction. It should be noted that citric acid pretreatment was essential for confined catalyst activation. The activation treatment could dramatically enhance catalyst surface acidity, especially a large number of strong acid sites were supplemented, resulting in significantly enhancement of catalytic activity at high temperature. Furthermore, it could also accelerate reduction of Ce 4+ to Ce 3+ and generate more active oxygen species, which resulted in a significant improvement in its low-temperature catalytic activity. Owning with strong surface acidity as well as framework confinement effect, the unique ordered mesoporous TiO 2 framework could inhibit SO 2 adsorption and protect active sites from SO 2 attacking. Thus, the framework confined FW-CeW/OMT exhibited wide operating temperature window, good thermal stability, as well as strong sulfur resistance in NH 3 -SCR process.
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FUEL
·
2022
·
IF 8.035
Ruolan Li,Zongqian Wu,Ya Chen,Xingyan Liu,Weiwei Guo,Yumin Huang,Min Fu,Youzhou He
An efficient bifunctional porphyrin-based MOF is fabricated for photocatalytic hydrogen evolution and NO removal, in which the mixed Zr/Ti-oxo clusters are the metal nodes and uniformly distributed Pt nanoparticles (Pt NPs) are the co-catalysts. It is worth noting that the optimal Zr-MOF-s(Pt)(Zr/Ti)-R is obtained through replacing partial Zr(IV) with Ti(IV) in the original Zr-based porphyrin MOFs and in-situ generating confined Pt NPs with a relatively small size within the internal cavities. Compared with the majority of reported Zr-based porphyrin MOFs, the Zr-MOF-s(Pt)(Zr/Ti)-R exhibits an extremely high hydrogen evolution activity (2545.11 μmol·g −1 ·h −1 ) and NO removal rate (46.6 %) under visible light irradiation. The excellent photocatalytic performance should be ascribed to the reason that the mixed Zr/Ti-oxo cluster and the in-situ generated Pt NPs significantly promote the rate of charge transfer and separation. Moreover, the photocatalytic NO oxidation process was also monitored by in - situ DRIFTS, which indicates the Zr-MOF-s(Pt)(Zr/Ti)-R could realize the effective oxidation of NO and intermediates to the final product (NO 3 – ). This work provides us with a practical route to further improve the photocatalytic performance by synergistically modifying the original metal clusters to adjust the ligand-to-metal charge transfer efficiency and in-situ introducing metal nanoparticles to form Schottky junctions.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Junqi Cheng,Zhitao Han,Jiawei Li,Xinxiang Pan
Previous work proposed a one-stage wet scrubbing in situ combined with O3 oxidation for simultaneous removal of NO and SO2 from flue gas, and the results showed that wet scrubbing combined in situ with O3 injection could effectively improve O3 oxidant utilization efficiency. In this work, a follow-up research work was carried out to further explore the synergistic effect of dual oxidants of NaClO in the liquid phase and O3 in gas phase. The synergistic effects of O3/NO molar ratio and NaClO concentration in the circulating scrubbing solution on NOx removal performance was investigated systematically. The results showed that when molar ratio of O3/NO was 0.5 and NaClO concentration was 25 mM, NO could be oxidized completely and averaged NOx removal efficiency exceeded 70%. NOx concentrations in outlet gas and anion compositions in the scrubbed solution were analyzed, and the possible reaction paths of wet scrubbing NaClO solution in situ with O3 injection in denitration process were also discussed. When the solution pH was around 6, a relative balance between NOx oxidation and absorption might be achieved, resulting in a high NOx removal efficiency. The temperature of inlet flue gas imposed little impact on NOx removal efficiency due to the quick and efficient cooling effect by wet scrubbing. The increase of initial SO2 concentration led to a slight increase of NOx removal efficiency from 70 to 73.5%. A complete removal of SO2 could be achieved, but coexisting SO2 in flue gas would consume NaClO oxidant and shorten the reaction duration.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Youzhou He,Mingzuo Chen,Yao Jiang,Lei Tang,Jianning Yu,Ya Chen,Min Fu,Xuemei Tan,Jiajia Jing,Guizhi Zhang,Xingyan Liu
The modification of graphite carbonitride (g-C 3 N 4 ) is beneficial to increase its specific surface area and high quantum efficiency, thus improving its activity. Herein, the Yb 2 O 3 /g-C 3 N 4 composites were adjusted through dual regulation synergistically (nanostructure design of g-C 3 N 4 and addition of lanthanide oxides Yb 2 O 3 ) to improve the photocatalytic performance of hydrogen production and NO removal simultaneously. The as-prepared 1% Yb 2 O 3 /tubular g-C 3 N 4 could efficiently promote the photocatalytic hydrogen evolution (4071.763 μmol·g −1 ·h −1 ) and NO removal performance (54.20%), which was approximately 8.85 times and 32.01% higher respectively than that of bulk g-C 3 N 4 prepared by melamine (g-C 3 N 4 -M). The formation process of·O 2 - and·OH radicals and the oxidation process of NO had been systematically studied through ESR and in-situ DRIFTS , which proved that the coupling of tubular g-C 3 N 4 with Yb 2 O 3 had a positive effect. This work provided a novel strategy for dual regulation (adjust morphology and metal oxide introduction) synergistically design of bifunctional photocatalysts to enhance H 2 production and NO removal simultaneously.
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ChemCatChem
·
2021
·Vol. 13
·期 7
·1834-1846
·
IF 5.686
Ruihuan Jiang,Shaomian Liu,Liang Li,Yongjun Ji,Huifang Li,Xiangfeng Guo,Lihua Jia,Ziyi Zhong,Fabing Su
Graphical Single Ir atoms : In the CO+NO reaction, the catalyst with single-sited Ir atoms (0.28 wt %) anchored on a mesoporous WO 3 (Ir 1 /mesoporous-WO 3 ) showed much higher NO conversion and N 2 selectivity under oxygen-rich conditions than the catalysts supported with Ir nanoparticles on the same catalyst support (Ir NPs/mesoporous-WO 3 ) and on a non-mesoporous WO 3 (Ir/non-mesoporous-WO 3 ). Under oxygen-rich conditions, achieving a selective and efficient reduction of NO by CO is always challenging. Here, we report the synthesis of the catalyst consisting of single Ir atoms anchored on mesoporous WO 3 (denoted as Ir 1 /m-WO 3 ) using a facile template method followed by wet impregnation. X-ray diffraction and transmission electron microscope studies indicated that the Ir atoms were distributed uniformly on the internal surface of m-WO 3 . When tested for the reduction of NO by CO, the Ir 1 /m-WO 3 catalyst with a low Ir loading of 0.28 wt % exhibited excellent catalytic performance in the presence of 2 vol % O 2 (volume ratio of CO to O 2 being 1 : 10), achieving a NO conversion of 73 % and N 2 selectivity of 100 % at 350 °C. In particular, its turnover frequency (TOF) value reached 0.30 s −1 at 200 °C, which is six times higher than that of the catalyst with Ir nanoparticles supported on mesoporous WO 3 (0.05 s −1 ). The superior catalytic performance of Ir 1 /m-WO 3 is attributed to the formation of the isolated Ir atoms and the more newly generated Ir-WO 3 interfaces that can promote the adsorption and activation of NO, and the presence of accessible mesopores in m-WO 3 that facilitates the mass transfer of NO and CO. This study brings a new fundamental understanding of active sites in Ir-based catalysts for the CO+NO reaction and provides a new way to the design and synthesis of single-atom catalysts, especially precious metal catalysts for emissions control.
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MOLECULAR PHARMACEUTICS
·
2021
·
IF 4.939
Zhiting Sun,Xiaoxiao Wang,Jing Liu,Zhihong Wang,Weiwei Wang,Deling Kong,Xigang Leng
Photodynamic therapy (PDT) is promising for clinical cancer therapy; however, the efficacy was limited as an individual treatment regimen. Here, an approach synergistically combining PDT and nitric oxide (NO) gas therapy along with destruction of the tumor extracellular matrix (ECM) was presented to eliminate cancer. Specifically, the NO donor l-arginine (l-Arg) and the photosensitizer indocyanine green (ICG) were co-encapsulated in poly(lactic-glycolic acid) (PLGA) nanoparticles and then loaded into the poly(ε-caprolactone)-poly(ethylene glycol)-poly(ε-caprolactone) (PCL–PEG–PCL) hydrogel to develop an injectable, thermosensitive dual drug delivery system (PLGA@ICG@l-Arg/Gel). Significantly, reactive oxygen species (ROS) produced by PLGA@ICG@l-Arg/Gel under near-infrared (NIR) light irradiation could not only result in the apoptosis of cancer cells but also oxidize l-Arg to generate NO, which could suppress the proliferation of cancer cells. Moreover, ROS could further oxidize NO to generate peroxynitrite anions (ONOO–). ONOO– could activate matrix metalloproteinases (MMPs), which notably degraded collagen in ECM so as to damage the tumor microenvironment. PLGA@ICG@l-Arg/Gel significantly increased the antitumor efficacy against highly malignant 4T1 tumors in mice. Taken together, PLGA@ICG@l-Arg/Gel is a multifunctional platform that provides a novel strategy for cancer treatment with cascade amplification of the ROS oxidation effect, which holds great potential in clinical translation.
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