Bioactive Materials
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2023
·
IF 18.9
Qiongyu Qin,Ming Yang,Yu Shi,Haijing Cui,Chunshu Pan,Wenzhi Ren,Aiguo Wu,Jianqing Hu
Currently, precise ablation of tumors without damaging the surrounding normal tissue is still an urgent problem for clinical microwave therapy of liver cancer. Herein, we synthesized Mn-doped Ti MOFs (Mn–Ti MOFs) nanosheets by in-situ doping method and applied them for microwave therapy. Infrared thermal imaging results indicate Mn–Ti MOFs can rapidly increase the temperature of normal saline, attributing to the porous structure improving microwave-induced ion collision frequency. Moreover, Mn–Ti MOFs show higher 1 O 2 output than Ti MOFs under 2 W of low-power microwave irradiation due to the narrower band-gap after Mn doping. At the same time, Mn endows the MOFs with a desirable T 1 contrast of magnetic resonance imaging (r 2 /r 1 = 2.315). Further, results on HepG2 tumor-bearing mice prove that microwave-triggered Mn–Ti MOFs nearly eradicate the tumors after 14 days of treatment. Our study offers a promising sensitizer for synergistic microwave thermal and microwave dynamic therapy of liver cancer.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Ao Zhang,Zhongqing Jiang,Shaoda Zhang,Penghua Lan,Naihua Miao,Weiheng Chen,Ning Huang,Xiaoning Tian,Yangjie Liu,Zhongyu Cai
We report the development of non-noble transition metal sulfide catalysts Mn-CuS-x for high-efficiency and selective H 2 O 2 production. In this study, we synthesized Mn-CuS-x with coral-shaped hierarchical porous structure through one-pot hydrothermal reaction. The Mn-CuS-x possesses large specific surface area with plenty of crystalline defects via heteroatom doping of Mn. The Mn-CuS-x kinetically favored 2e − pathway over 4e − pathway, resulting in high selectivity (>92%) to H 2 O 2 production and high H 2 O 2 concentration (∼24.5 mM at 0.6 V vs. RHE) within 3 h for the optimized Mn-CuS-2 catalysts (synthesized with a molar ratio of 1:3:8 (MnCl 2 ·4 H 2 O: CuCl 2 ·2 H 2 O: C 2 H 5 NS)). The Mn-CuS-2 showed excellent stability, indicating that the Mn-CuS electrocatalysts can simultaneously achieve both high stability and enhanced H 2 O 2 production. Our first-principles calculations further confirmed that the heteroatom Mn doping to CuS thermodynamically makes the 2e – -ORR pathway more favorable. This study provides a green, low-cost, and efficient route to produce H 2 O 2 , which is very promising for generating chemicals and liquid fuels.
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Analytical Methods
·
2019
·Vol. 11
·期 8
·1111-1124
·
IF 2.378
Xiaoheng Qi,Huiming Tian,Xueming Dang,Yaofang Fan,Yaobin Zhang,Huimin Zhao
Metal–organic frameworks (MOFs) with a metal coordination structure mimicking that of enzymes have been widely applied in the sensing field for bioassays, and most of the reports focus on single-metal MOFs. However, bimetallic MOFs have fascinating catalytic capabilities due to their bimetallic coordination. Herein, a two-dimensional sheet-like bimetallic Co/Mn-based MOF (Co/Mn-MOF) with peroxidase-like activity was synthesized through a one-step hydrothermal method to accelerate the decomposition of H2O2 with the generation of ˙OH, which further oxidized the classic chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB) into oxTMB. The Michaelis–Menten constants (Km) and maximum initial velocities (Vmax) of the catalyst were found to be 0.27 mM and 1.64 × 10−7 M s−1 for TMB and 0.24 mM and 5.80 × 10−7 M s−1 for H2O2, respectively. Accordingly, we successfully utilized Co/Mn-MOF-1-1-150 to establish a colorimetric detection platform for the detection of H2O2. A linear absorbance response ranging from 1 to 100 μM with the limit of detection of 0.85 μM (S/N = 3) was obtained under the optimized conditions. The LOD of our catalyst is comparable to that of other MOF-based enzyme mimics for colorimetric detection; this can be ascribed to the synergistic catalytic effect between its two metals, its two-dimensional structure with a small diffusion barrier for the substrate molecules, and large exposed surface area. More importantly, using the proposed sensing method, the determination of H2O2 released by living cells and in spiked water samples was achieved. This revealed that the as-prepared bimetallic Co/Mn-MOF could be a promising candidate as a catalytic material due to its peroxidase activity.
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高影响因子
JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Qin Wang,Yejian Xue,Shanshan Sun,Shanshan Yan,He Miao,Zhaoping Liu
Facile synthesis of high efficient bi-functional oxygen catalysts is important for large-scale application of rechargeable metal-air batteries . Herein, an ethanol-water mediated co-precipitation approach is applied to fabricate Co–Mn–Ni (CMN) ternary spinel oxides with uniform 1D structure. Their catalytic activities toward the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are investigated by the rotating ring-disk electrode (RRDE) techniques. The ternary spinel oxide with the Co/Mn/Ni atomic ratio of 2:3:1 (CMN-231) exhibits the best bi-functional activities among the as-prepared ternary, binary and unitary spinel oxides (△E is as low as 0.88 V), which can be attributed to its reasonable element composition , mesoporous nanorod structure, strong oxygen-adsorption ability and good charger-transfer capability. In addition, the CMN-231 catalyst demonstrates a strong stability during long-term operation. This well-designed catalyst is applied in a homemade zinc-air battery, and exhibits good charge–discharge performances (voltage gap is 0.9 V at 50 mA cm −2 ) and remarkable cycling stability.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2018
·
IF 3.779
Dmitrii Rakov,Yuzhi Li,Siqi Niu,Ping Xu
Recently reported transition metal phosphosulfide (MPS 3 or MPS) nanosheets (NSs) demonstrated outstanding activity towards hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), and proper doping of a second transition metal might even enhance the catalytic activity. By considering the oxophilicity of the doping element, here we demonstrate the Mn (with higher oxophilicity) and Ni (with lower oxophilicity) doping of Ni 1- x Mn x PS 3 and Mn 1- x Ni x PS 3 NSs on their HER and OER activity in alkaline solution. It is found that non-substituted NiPS 3 NSs show better catalytic activity than their Mn-doped samples. On the contrary, Ni doping into MnPS 3 NSs significantly improves the electrocatalytic performance. This work may substantially expand the understanding of the role of elemental oxophilicity on the electrochemical water splitting activities of Ni/Mn based catalysts.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Yuying Zhang,Na Li,Lianmei Chen,Fangrui Yu,Xueru Sheng,Jian Zhang,Qingwei Ping,Hongbin Li
Laccase immobilization is an effective way to realize the industrial application of laccase, but the loss of immobilized laccase activity is serious, which is an urgent problem to be solved. In this study, a novel laccase immobilization material was prepared by mixing waste Mn–Cu-loaded activated carbon with cellulose solution and regenerated in hydrochloric acid solution, which significantly improved the immobilized laccase activity. The optimum immobilization conditions (T, pH and initial laccase concentration) of Mn–Cu-AC/cellulose beads (Mn–Cu-ACC) for laccase were studied by the response surface method. Under the optimum conditions (T = 43 °C, pH = 4.0 and c = 6.8 g L−1), immobilized laccase (Laccase@Mn–Cu-ACC) showed excellent performance in terms of pH stability, thermostability and storage stability. And the enzyme activity of the laccase immobilized on the Mn–Cu-ACC carrier remarkably increased by 29.6% compared to that of the ACC. At last, the Laccase@Mn–Cu-ACC was used for the degradation of bisphenol A (BPA). Under the optimum conditions (t = 5.5 h, T = 45 °C, pH = 4.0 and initial cBPA = 70 mg L−1), the removal rate of BPA reached 72.3% in the first cycle, and after 5 cycles of reusing the immobilized laccase, the relative removal rate of BPA was retained at 53.2% of the initial removal rate. This study developed a new type of immobilized laccase carrier and provided a new path for the application of waste heavy metal loaded activated carbon.
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高影响因子
FOOD CHEMISTRY
·
2017
·
IF 4.529
Wengang Zhang,Yong Han,Xiumei Chen,Xueli Luo,Jianlong Wang,Tianli Yue,Zhonghong Li
A Mn-doped ZnS quantum dots (QDs) based nanosensor for selective phosphorescent determination of patulin (PAT) was synthesized with 6-hydroxynicotinic acid (6-HNA) as dummy template via a surface molecular imprinting sol–gel process. FTIR and XRD indicated the successful graft of molecularly imprinted polymer (MIP) onto crystal QDs. Binding tests revealed that the MIP-QDs presented higher selectivity, adsorption capacity and mass transfer rate than non-imprinted polymers, demonstrating a specific recognition for PAT among competitive mycotoxins and its analogues with the imprinting factor of 2.02. The MIP-QDs could recognize PAT in a linear range of 0.43–6.50 μmol L −1 with a detection limit of 0.32 μmol L −1 and a correlation coefficient (R 2 ) of 0.9945. Recoveries of 102.9–127.2% with relative standard deviations <4.95% were achieved in apple juice samples which were in good agreement with high-performance liquid chromatography (HPLC) (P > 0.05). The results indicated a simple phosphorescent nanosensor for PAT detection in complex matrix.
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PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2017
·
IF 5.401
Zhi-Qiang Zhou,Ren Yan,Jie Zhao,Li-Yun Yang,Ji-Lei Chen,Yan-Jun Hu,Feng-Lei Jiang,Yi Liu
The pollution of Hg 2+ is one of the most serious problems to human health due to their high toxicity, mobility, difficulty in degradation and ability of accumulation in ecological systems. Thus, it is of great importance to develop highly selective and sensitive probe for detecting Hg 2+ in aquatic ecosystems. Here we propose a new turn-on strategy for specific recognition and detection of Hg 2+ . Mn-doped ZnSe quantum dots (QDs) with small size (2.1 nm) were prepared and adopted as probe, the small size of doped QDs makes the replacement of Mn 2+ by Hg 2+ accessible, which eliminates the fluorescence quenching effect of superficial Mn 2+ on Mn-doped ZnSe QDs. Different from traditional semiconductor nanocrystals based turn-off probe for detecting Hg 2+ , we realize a turn-on strategy for the selective detection of Hg 2+ by Hg 2+ -Mn 2+ replacement using semiconductor nanocrystals (Mn-doped ZnSe QDs). This turn-on mechanism was verified by fluorescence spectra, ICP-AES and XPS. In the absence of Hg 2+ , Mn-doped ZnSe QDs possessed low fluorescence intensity. With the addition of Hg 2+ , the fluorescence intensity around 600 nm increased dramatically. Our Mn-doped ZnSe QDs exhibits excellent selectivity and sensitivity for Hg 2+ . The limit of detection is 7.0 nM, which is lower than the mercury toxic level defined by the U.S. Environmental Protection Agency (10 nM). The result of Hg 2+ detection in real samples indicates the feasibility and sensitivity of our probe for application in environmental samples.
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高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2013
·
IF 2.145
Wei-guo Pan,Jie-nan Hong,Rui-tang Guo,Wen-long Zhen,Hong-lei Ding,Qiang Jin,Cheng-gang Ding,Shi-yi Guo
MnO x –CuO x /TiO 2 and MnO x –CuO x /Al 2 O 3 catalysts were prepared by sol–gel method and used for low temperature selective catalytic reduction of NO with NH 3 . The results showed that MnO x –CuO x /TiO 2 had better catalytic activity and SO 2 resistance than MnO x –CuO x /Al 2 O 3 in the temperature range of 100–250 °C. The properties of the catalysts were characterized by using XRD, N 2 adsorption, temperature programmed reduction (H 2 -TPR) and temperature programmed desorption (NH 3 -TPD). It was found that the support has a great impact on the acidity of catalyst; TiO 2 and Al 2 O 3 can promote the formation of Lewis acid sites and Brönsted acid sites respectively.
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高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Yue Yin,Yanming Xu,Ya-Nan Luan,Zhuo Zhao,Yihua Xiao,Changqing Liu
A novel porous Fe-Mn chitosan bead (PFMB) was fabricated through the freeze-drying technique for the enhanced oxidation and adsorption of arsenite (As(Ⅲ)) from aqueous solution. The porous internal structure of PFMB provided a significantly higher As(Ⅲ) oxidation and adsorption rate than solid Fe-Mn chitosan bead (FMB). The experimental results showed that FMB and PFMB exhibited the theoretical maximum As(Ⅲ) adsorption capacities of 27.42 and 49.80 mg/g, respectively. The real-time oxidation and adsorption progress of As(Ⅲ) onto PFMB was deeply evaluated: PFMB effectively oxidized As(Ⅲ) to As(Ⅴ) and the generated As(Ⅴ) was subsequently adsorbed. The operational parameters (initial pH, adsorbent dosage, ionic strength, and HA concentration) were thoroughly investigated and had no significant influence on As(Ⅲ) removal by PFMB. Finally, the regeneration experiment showed that PFMB can be easily regenerated and the recycled PFMB can successfully remove As(Ⅲ) in the following 5 cycles. Column experiments suggested that the column device could effectively remove the As(Ⅲ) in more than 3830 bed volume with the influent velocity at 0.5 mL/min before effluent concentration reached 0.05 mg/L. These results revealed the enhanced oxidation and adsorption performance of As(Ⅲ) onto PFMB and provided a reference for the future application of PFMB in arsenic-contaminated water treatment.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhigen Li,Mengfan Zhou,Shuqin Wang,Baowei Hu
Uranium (U(VI)) removal from nuclear-contaminated water is still an obstacle that needs to be solved quickly. Herein, looking for efficient, fast, and highly selective separation of U(VI) versatile material is of great significance. In this study, a novel Ce/Mn bimetallic modified aminated MOF material UiO-66-NH 2 was synthesized through solvothermal reaction by using ZrOCl 2 ·8H 2 O as a sacrificial template, which was employed as an adsorbent in radioactive remediation. The characterization of the adsorbent Ce/Mn-UiO-66-NH 2 was investigated by XRD, FTIR, SEM, and BET and the results indicated that Zr in UiO-66-NH 2 had been partially replaced by Ce/Mn successfully. Through batch adsorption experiments, we found that the maximal capture capacity of the produced adsorbent for U(VI) was 1218.78 mg/g at 313 K, and the elimination process fitted well with pseudo-second-order kinetic model and the Langmuir isotherm model. The thermodynamic parameters indicate that the adsorption process of U(VI) was endothermic and spontaneous which was regulated by chemisorption. After 5 times recycling, the removal rate still exceeded 83.5 %, indicating that Ce/Mn-UiO-66-NH 2 was a promising adsorbent that can effectively remove U(VI) in radioactive wastewater. The increased adsorption capacity was proposed attributed to complexation and electrostatic attraction between the radionuclides and the introducing functional groups as well as Ce or Mn ions. This study provides a reference value for radioactive wastewater remediation.
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高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·Vol. 39
·期 1
·e7959
·
IF 3.7
Zhuoqin Li,Minghui Ma,Zhiyin Xiao,Xiujuan Jiang,Xinlei Xu,Hailong Wang,Peter C. Ford,Xiaoming Liu
Five novel manganese (I) tricarbonyl complexes were synthesized by the reaction of Mn (CO) 5 Br with quinoline-2-carboxaldehyde and different anilines. The IR, UV, and myoglobin results indicate that these complexes can be used as photoCORMs (photo photoinduced carbon monoxide releasing molecules) activated by red light. The visible range spectra display strong charge transfer (CT) bands, the maxima of which are sensitive to the ligand substituents. Density functional theory (DFT) and time-dependent density functional theory (TDDFT) computations show that these CT transitions are admixtures of metal-to-ligand and aniline-to-quinoline charge transfers and that increasing the electron-donating ability on the aniline functionality can lead to shifts in the absorption bands of the corresponding compounds to longer wavelengths and to enhanced band intensities, thus enhancing their photoactivity. Photolysis of these complexes in aerobic solution leads to CO photodissociation followed by oxidation of the Mn(I) center to Mn(II).
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