ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Liying Hao,Jikui Sun,Qingyin Wang,Haijiao Xie,Xiangui Yang,Qiang Wei
As an atom-economical reaction, the direct generation of dimethyl carbonate (DMC) and ethylene glycol (EG) via the transesterification of CH3OH and ethylene carbonate (EC) has several promising applications, but the exploration of carriers with high specific surface areas and novel heterogeneous catalysts with more basic sites remains a long-standing research challenge. For this purpose, herein, a nitrogen-doped mesoporous carbon (NMC, 439 m2/g) based K–O2 Lewis base catalyst (K–O2/NMC) with well-dispersed strongly basic sites (2.23 mmol/g, 84.5%) was designed and synthesized. The compositions and structures of NMC and K–O2/NMC were comprehensively investigated via Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, N2 adsorption–desorption, CO2 temperature-programmed desorption, and contact angle measurements. The optimal structural configuration and electron cloud distribution of the K–O2/NMC catalyst were simulated using first-principles calculations. The electron transfer predominantly manifested as a flow from K–O to C–O/C–N, and the interatomic interactions between each atom were enhanced and exhibited a tendency for a more stable state after redistribution. Furthermore, the adsorption energies (Eads) of CH3OH at K–O–O and K–O–N sites were −1.4185 eV and −1.3377 eV, respectively, and the O atom in CH3OH exhibited a stronger adsorption tendency for the K atom at the K–O–O site. Under the optimal conditions, the EC conversion, DMC/EG selectivity, and turnover number/frequency were 80.9%, 98.6%/99.4%, and 40.5/60.8 h–1, respectively, with a reaction rate constant (k) of 0.1005 mol/(L·min). Results showed that the heterogeneous K–O2/NMC catalyst prepared herein greatly reduced the reaction cost while guaranteeing the catalytic effect, and the whole system required a lower reaction temperature (65 °C), a shorter reaction time (40 min), and a lower catalyst amount (2.0 wt % of EC). Therefore, K–O2/NMC can be used as a catalyst in different transesterification reactions.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2016
·
IF 5.393
Ting Liu,Lucheng Xue,Xin Guo,Jia Liu,Yu Huang,Chuguang Zheng
The reaction mechanisms of a mixture gas of HCl, O2, and SO2 in Hg0 adsorption on α-Fe2O3(001) surface are clarified by a group of adsorption experiments and theoretical calculations based on the density functional theory. The role of O2 in removing Hg0 is greatly influenced by the reaction temperature, meanwhile, the O atom coverage could affect the adsorption performance of Hg0. The dissociated O2 competes with the active sites of Cl species on Fe surface at low temperature, however, at medium temperature HCl and O2 could simultaneously facilitate the Hg0 transformation. Combined with the theoretical calculations, the role of SO2 and the probable pathways in removing Hg0 are discussed. Lower concentration of SO2 as well as HCl could dissociate on α-Fe2O3(001) surface, and the intermediates combine with gaseous Hg0, forming mercury–sulfur, mercury–chlorine compounds, and so forth. In addition, the different concentrations of SO2 are also discussed, and the corresponding X-ray photoelectron spectroscopy analysis on contrasted samples is conducted to research the morphological characterization, providing a reliable basis for judging the probable pathways of Hg0 transformation.
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Small
·
2016
·Vol. 12
·期 39
·5477-5487
·
IF 8.315
Zhifang Ma,Mengchao Zhang,Xiaodan Jia,Jing Bai,Yudi Ruan,Chao Wang,Xuping Sun,Xiue Jiang
Local hypoxia in tumors, as well as the short lifetime and limited action region of 1 O 2 , are undesirable impediments for photodynamic therapy (PDT), leading to a greatly reduced effectiveness. To overcome these adversities, a mitochondria-targeting, H 2 O 2 -activatable, and O 2 -evolving PDT nanoplatform is developed based on Fe III -doped two-dimensional C 3 N 4 nanofusiform for highly selective and efficient cancer treatment. The ultrahigh surface area of 2D nanosheets enhances the photosensitizer (PS) loading capacity and the doping of Fe III leads to peroxidase mimetics with excellent catalytic performance towards H 2 O 2 in cancer cells to generate O 2 . As such tumor hypoxia can be overcome and the PDT efficacy is improved, whilst at the same time endowing the PDT theranostic agent with an effective T 1 -weighted in vivo magnetic resonance imaging (MRI) ability. Conjugation with a mitochondria-targeting agent could further increase the sensitivity of cancer cells to 1 O 2 by enhanced mitochondria dysfunction. In vitro and in vivo anticancer studies demonstrate an outstanding therapeutic effectiveness of the developed PDT agent, leading to almost complete destruction of mouse cervical tumor. This development offers an attractive theranostic agent for in vivo MRI and synergistic photodynamic therapy toward clinical applications.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Renjie Deng,Huajie Liu,Haishuai Cui,Yao Tian,Hai Yang
In this work, we have developed a green method for the preparation of para-nitrotoluene through the catalytic nitration of toluene with nitrogen dioxide (NO2) under the promotion of dioxygen (O2). The experimental results reveal that the dealumination of Hβ zeolite has a significant effect on the catalysis of the developed NO2–O2–acetic anhydride (Ac2O) system, in which the conversion of toluene is 78.1% and the selectivity to para-nitrotoluene is 71.8%. Furthermore, the nature of different dealuminated catalysts was investigated by nitrogen adsorption–desorption analysis, X-ray diffraction (XRD), Fourier-transform infrared (FT-IR), thermal gravimetric analysis (TGA), inductively coupled plasma (ICP), ammonia temperature-programmed desorption (NH3-TPD), pyridine adsorbed Fourier-transform infrared (Py-FT-IR), scanning electron microscopy (SEM) and 27Al magic-angle spinning nuclear magnetic resonance (27Al MAS NMR) techniques. The results of characterization indicate that the structure of the Hβ zeolite still remains and that of Al species in the extra-framework is preferentially removed after acid treatment. Based on the combined results of catalytic characterization and DFT calculation, a feasible reaction mechanism of improved para-selectivity in toluene nitration was suggested for the NO2–O2–Ac2O system.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Leilei Hou,Siyang Yan,Liping Liu,Jiaxu Liu,Guang Xiong
The TS-1 microsphere was facilely prepared via a direct spray drying of the mixture containing the nanocrystal TS-1 and mother liquor. The calcined TS-1 zeolites possess a hollow structure and numerous intercrystalline mesopores, which may facilitate the diffusion properties. Au nanoparticles were loaded on TS-1 support by utilizing a deposition–precipitation process to prepare the Au/TS-1-M catalysts for propylene epoxidation in the presence of H 2 and O 2 conditions. The effects of the Ti and Au loadings on the structure, porosity, morphology, and catalytic performances of the Au/TS-1 catalysts have been investigated by various techniques. Under the optimized synthesis conditions (Si/Ti molar ratio = 57, 0.49 wt% Au), a propylene conversion of 6.1 % and a PO selectivity of 91.7 % were obtained on the Au/TS-1 catalyst. A PO formation rate of 186.8 g PO ·kg cat. −1 ·h −1 was achieved at the 20th hour.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xueyi Zhang,Wenshuang Sun,Yue Wang,Zhen Li,Xianqiang Huang,Tielong Li,Haitao Wang
In this study, we prepared a micron zero-valent iron/ N -doped graphene-like biochar (mZVI/NGB) composite using a mechanochemical method for tetracycline (TC) degradation through O 2 activation. The mZVI and NGB components formed a strong coupling catalytic system, with mZVI acting as an electron pool and NGB as a catalyst for H 2 O 2 generation. Under circumneutral pH (5.0–6.8), the mZVI/NGB composite exhibited exceptional TC removal efficiency, reaching nearly 100 % under optimal conditions. It also showed good tolerance to co-existing anions, such as Cl - , SO 4 2- , and humic acid. Further studies found that the TC degradation mechanism was mainly ascribed to the non-radical pathway ( 1 O 2 and electron transfer), and the Fe 2+ /Fe 3+ redox cycle on the composite's surface also played a crucial role in maintaining catalytic activity. This research contributes to the development of advanced materials for sustainable and effective water treatment, addressing pharmaceutical pollutant contamination in water sources.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiahui He,Zhenlong Li,Jueying Chen,Jiaxin Wang,Lipeng Qiao,Baolin Guo,Juan Hu
It is still challenging to design stimuli-responsive smart hydrogel dressing to promote bacteria-infected diabetic wound healing from the whole healing stage by intelligently responding to external stimuli or wound microenvironment. In addition, nitric oxide (NO) and oxygen (O 2 ) have been shown to accelerate diabetic wound healing by promoting angiogenesis and alleviating hypoxia. A series of NIR/glucose stimuli-responsive multifunctional smart hydrogels with NO/O 2 dual gas-releasing properties was designed based on N-carboxyethyl chitosan-grafted-phenylboronic acid (CECP), oxidized dextran (OD), ε-polylysine (EPL)-coated manganese dioxide (EMn), and β-cyclodextrin-reduced graphene oxide/N, N’-di-sec-butyl-N, N’-dinitroso-1,4-phenylenediamine (rGB) via dual dynamic crosslinking to promote bacteria-infected diabetic wound healing. The added rGB and EMn as photothermal agents rapidly kill bacteria through photothermal therapy. Meanwhile, rGB endows CECP/OD/EMn/rGB hydrogels to release NO under NIR stimulation to promote angiogenesis. Nanozyme EMn with catalase (CAT)/superoxide dismutase (SOD)-like activity can scavenge ROS and release O 2 to alleviate hypoxia and oxidative stress. The phenylboronic acid in CECP forming phenylboronate ester structure endows hydrogel with glucose-controlled release of doxycycline. NIR/glucose stimuli-responsive CECP/OD/EMn/rGB hydrogels with NO/O 2 dual gas-releasing property in a full-thickness skin wound-infected diabetic model reduced the inflammation, promoted wound contraction, collagen deposition, angiogenesis, and alleviated wound hypoxia, providing new ideas for treating bacteria-infected diabetic wounds.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Xichen Sun,Pengfei Wang,Liuyan Tang,Ningning Li,Yan-Ru Lou,Yuezhou Zhang,Peng Li
An effective method capable of simultaneously providing antibacterial activity, blood glucose regulation, and angiogenesis promotion for healing bacteria-infected diabetic wounds is not reported to date, but urgently required. In this study, a hydrogel composite ( γ -PGA/PDA/GOx/WO x (PPGW)), endowed with these desired attributes is fabricated by incorporating polydopamine (PDA), glucose oxidase (GOx), and tungsten oxide (WO x ) nanowires into the poly( γ -glutamic acid) ( γ -PGA) framework. The exceptional photothermal conversion properties of PDA facilitated notable antibacterial effects on bacteria-infected diabetic wounds; GOx regulated high blood glucose by consuming glucose and generating hydrogen peroxide (H 2 O 2 ); while WO x nanowires displayed remarkable photocatalytic abilities, converting H 2 O 2 into oxygen (O 2 ) when exposed to 808-nm near-infrared radiation. Density functional theory calculations and experiments are conducted to confirm the mechanism of WO x -mediated photocatalytic degradation of H 2 O 2 to produce O 2 . These transformations aided in alleviating the hypoxic conditions in wounds associated with diabetes, expediting angiogenesis, and fostering cell crawling and proliferation. Consequently, the multifunctional hydrogel dressing PPGW, featuring photothermal, antibacterial, and enzyme-catalyzed activity reduces hyperglycemia at the wound site. Moreover, photocatalytic O 2 production represents a promising strategy for addressing chronic bacteria-infected diabetic wounds.
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Advanced Healthcare Materials
·
2024
·
IF 10
Ming-Xuan Liu,Yan-Chao Liu,Yu-Ting Cai,Ying-Ying Gu,Ya-Qi Zhu,Nan Zhang,Wei-Zhong Zhu,Yong-Hong Liu,Lei Yu,Qi-Tao Zhang,Xiao-Ling Zhang
Hypoxia can aggravate tumor occurrence, development, invasion, and metastasis, and greatly inhibit the photodynamic therapy (PDT) effect. Herein, carbon nitride (CNs)-based DNA and photosensitizer co-delivery systems (BPSCNs) with oxygen-producing functions are developed to address this problem. Selenide glucose (Seglu) is used as the dopant to prepare red/NIR-active CNs (SegluCNs). The tumor-targeting unit Bio-PEG 2000 is utilized to construct BPSCNs nanoparticles through esterification reactions. Furthermore, DNA hydrophobization is realized via mixing P53 gene with a positively charged mitochondrial-targeted near-infrared (NIR) emitting photosensitizer (MTTPY), which is encapsulated in non-cationic BPSCNs for synergistic delivery. Ester bonds in BPSCNs@MTTPY-P53 complexes can be disrupted by lipase in the liver to facilitate P53 release, upregulated P53 expression, and promoted HIF-1α degradation in mitochondria. In addition, the oxygen produced by the complexes improved the hypoxic microenvironment of hepatocellular carcinoma (HCC), synergistically downregulated HIF-1α expression in mitochondria, promoted mitochondrial-derived ferroptosis and enhanced the PDT effect of the MTTPY unit. Both in vivo and in vitro experiments indicated that the transfected P53-DNA, produced O 2 and ROS by these complexes synergistically led to mitochondrial-derived ferroptosis in hepatoma cells through the HIF-1α/SLC7A11 pathway, and completely avoiding PDT resistance caused by hypoxia, exerting a significant therapeutic role in HCC treatment.
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Kexin Yang,Zhijia Song,XiaoXiao Fu,Wei Yan,Tao Zhang,Yiwei Hua,Haixin Lin,Qin Kuang,Zhaoxiong Xie
The photocatalytic direct one-step two-electron (2e-) oxygen reduction reaction (ORR) holds great potential in efficient H2O2 synthesis. However, it is still a significant challenge to design photocatalysts for achieving high-efficiency H2O2 production via this direct one-step 2e- ORR pathway. To address this, we have constructed a Z-scheme BAIO/C3N4 heterojunction by in situ growing Ba2AgIO6 (BAIO) on the surface of C3N4 nanosheets. Under visible light irradiation, the optimal sample, with a BAIO:C3N4 mass ratio of 1:1.5, exhibited a remarkable H2O2 yield of up to 535.9 μmol g-1 h-1, which is 8.8 times higher than that of pure C3N4. This enhancement is attributed to the improved charge separation and migration efficiency facilitated by the enhanced internal electric field (IEF) in BAIO/C3N4 heterojunction. Furthermore, the heterojunction altered the O2 adsorption configuration to the Yeager-type, promoting a more efficient and selective direct one-step 2e- ORR for H2O2 production. This study highlights the importance of regulating the reaction pathway to enhance photocatalytic H2O2 production activity and offers a new insight for designing highly active photocatalysts.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 21
·7378-7385
·
IF 5.721
Mengna Ding,Fengyan Shi,Huijuan Zhu,Yuping Yang,Jiahui Zhong,Liulin Luo,Yuning Huo,Hexing Li
A hybrid Cu2O/TiO2 composite loaded on a Cu mesh (Cu2O/TiO2@Cu mesh) was developed via a supercritical solvothermal route. A uniformly distributed Cu2O/TiO2 p–n hetero-junction was stably coated on a Cu mesh, benefiting the visible-light harvesting. In comparison to electrochemistry and visible-light photocatalysis, the photoelectrochemistry process on the photoanode of the Cu2O/TiO2@Cu mesh presented improved bacterial inactivation activity for Acinetobacter baumannii. By means of the main active species of ˙O2− radicals, the photoelectrocatalytic process on the Cu2O/TiO2@Cu mesh also realized complete leakage of K+ ions, much stronger mineralization of the cell membrane and more efficient elimination of the self-recovery function, finally leading to cell death. In comparison, the electrochemistry process only led to the leakage of K+ ions without inactivation of bacteria, and the visible-light photocatalysis process induced partial leakage of K+ ions and cell mineralization after the death of most bacteria.
研究领域:
环境科学
·
材料科学
·
微生物学
·
光电催化
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 9
·1-16
·
IF 2.4
Hu Rui,Wang Haiyin,Luo Jiahui,Song Jianjun,Jia Haiyuan
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have been proven to be an effective method for the removal of tetracycline in water. In this study, the Co 3 O 4 /molecular sieve catalyst synthesized by the incipient wetness impregnation method was used for PMS activation. The effect of specific surface area on the catalytic performance of Co 3 O 4 /molecular sieve catalyst was investigated and analyzed in detail by characterization techniques. In the Tetracycline hydrochloride (TCH) degradation experiment, the Co 3 O 4 /13X catalyst exhibited the highest specific surface area (490.584 m 2 /g) and provide abundant active sites, enabling 98.0% TCH degradation within 30 min under optimal conditions (1.5 g catalyst, 0.3 mM PMS, pH 8.0, 25℃), with a reaction rate constant (k obs ) of 0.0977 min -1 . In addition, the degradation mechanism of TCH was explored using electron paramagnetic resonance (EPR) spectroscopy and quenching experiments. It was confirmed that free radicals (SO 4 •− , •OH, O 2 •− ) and non-free radical species ( 1 O 2 ) generated during the reaction play a crucial role in the degradation process of TCH. In summary, the Co 3 O 4 /13X catalyst, when activating PMS, exhibits a remarkable synergistic effect on the degradation of TCH, and shows good repeatability and environmental adaptability. This study provides valuable insights into the design and optimization of catalysts for degrading antibiotic pollutants in water treatment processes. Graphical
研究领域:
环境科学
·
催化
·
水处理
·
化学工程
·
污染物降解
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