Journal of Physical Chemistry C
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2020
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IF 4.189
Yubin Zhao,Xiao Zhang,Cong Xie,Wenbin Shi,Ping Yang,San Ping Jiang
Although inorganic cesium halide lead perovskite nanocrystals (NCs) exhibited tunable photoluminescence (PL), it is still a challenge for such NCs with multicolor and white emission for application. In this article, as-synthesized Mn:CsPbCl3 NCs were treated using an oleoamine solution of CdX2 (X = Cl, Br) to get a high PL quantum yield (PLQY) and stability. CdCl2 passivated the surface defects of Mn:CsPbCl3 NCs through anion exchange to get high PL intensity, especially to increase Mn emission. The PLQY of the sample was increased from 15 to 85% after ion exchange. Furthermore, the treatment of CdBr2 resulted in the appearance of a powerful blue emission peak, and the PLQY increased to 95.7%. The PL decay kinetics of samples was studied before and after treatment. Mn2+ emission in Mn:CsPb(Cl/Br)3 NCs was increased because of the reaction of CdBr2 and Mn:CsPbCl3 NCs. Interestingly, the tunable and bright white emission from Mn:CsPb(Cl/Br)3 NCs was obtained by controlling the amount of Br. The controlling of Mn emission plays an important role in changing the Commission Internationale de l’Eclairage color coordinates. Because of bright and tunable PL, the NCs may be used in white-light-emitting diodes.
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Nature Communications
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2020
·Vol. 11
·期 1
·1-8
·
IF 12.121
Feng Jiaqi,Gao Hongshuai,Zheng Lirong,Chen Zhipeng,Zeng Shaojuan,Jiang Chongyang,Dong Haifeng,Liu Licheng,Zhang Suojiang,Zhang Xiangping
Developing effective catalysts based on earth abundant elements is critical for CO 2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO ( j CO ) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N 3 site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a j CO of 14.0 mA cm −2 at a low overpotential of 0.44 V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher j CO of 29.7 mA cm −2 is obtained in an ionic liquid electrolyte at 0.62 V overpotential. In situ X-ray absorption spectra and density functional theory calculations demonstrate that the remarkable performance of the catalyst is attributed to the Mn-N 3 site, which facilitates the formation of the key intermediate COOH * through a lowered free energy barrier.
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Molecular Catalysis
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2020
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IF 3.687
Anwei Wang,WeiYou Zhou,Zhonghua Sun,Zhong Zhang,Zhihui Zhang,MingYang He,Qun Chen
Developing efficient heterogeneous catalytic systems based on easily available materials and molecular oxygen for the selective oxidation of alkylarenes is highly desirable. In the present research, NiMn hydrotalcite (Ni 2 Mn-LDH) has been found as an efficient catalyst in the oxidation of alkylarenes using molecular oxygen as the sole oxidant without any additive. Impressive catalytic performance, excellent stability and recyclability, broad applicable scope and practical potential for the catalytic system have been observed. Mn 3+ species was proposed to be the efficient active site, and Ni 2+ played an important role in stabilizing the Mn 3+ species in the hydrotalcite structure. The kinetic study showed that the aerobic oxidation of diphenylmethane is a first-order reaction over Ni 2 Mn-LDH with the activation energy ( E a ) and pre-exponential factor ( A 0 ) being 85.7 kJ mol −1 and 1.8 × 10 9 min −1 , respectively. The Gibbs free energy (Δ G ≠ ) was determined to be -10.4 kJ mol -1 K -1 for the oxidation based on Eyring-Polanyi equation, indicating the reaction is exergonic. The mechanism study indicated that the reaction proceeded through both radical and carbocation intermediates. The two species were then trapped by molecular oxygen and H 2 O or hydroxyl species, respectively, to yield the corresponding products. The present research might provide information for constructing highly efficient and stable active site for the catalytic aerobic oxidation based on available and economic material.
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 4
·2285-2294
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IF 3.591
Nannan Liu,Simin Shang,Dajun Shi,Qingrong Cheng,Zhiquan Pan
Thanks to the unique structure and properties of MOFs, a well-designed novel hollow ZnO/Mn-ZIF-67 composite photocatalyst was synthesized by a facile sonocrystallization approach successfully. The hollow ZnO/Mn-ZIF-67 composites exhibited higher photocatalytic activity in degrading Bismarck brown R than pure hollow ZnO spheres and Mn-ZIF-67. The optimal ZnO/Mn0.5-ZIF-67 showed the highest catalytic activity with 89.5% Bismarck brown R removal within 100 min. The improved photocatalytic activity of the composites could be mainly attributed to effective photogenerated charge separation and transfer through the coupled Z-scheme heterojunction between hollow ZnO spheres and Mn-ZIF-67. The composite photocatalyst exhibited obviously good stability and recyclability after recycling 4 times. Finally, a possible Z-scheme electron transfer mechanism was proposed based on the active radical trapping experiments and ESR which could explain the improved photocatalytic performance of the photocatalytic system. This work provides a promising approach to construct a direct Z-scheme heterojunction for the degradation of environmental pollutants.
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ACS Biomaterials Science & Engineering
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2020
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IF 4.152
Yijue Wang,Liqing Zou,Zhe Qiang,Jianhai Jiang,Zhengfei Zhu,Jie Ren
Radiotherapy (RT) is a major treatment method for non-small-cell lung cancer (NSCLC), and development of new treatment modality is now critical to amplify the negative effects of RT on tumors. In this study, we demonstrated a nanoparticle-loaded block copolymer micellar system for cancer hyperthermia treatment (HT) that can be used for synergistic therapy under alternating magnetic field (AMF) and radiation field. Block copolymer micelles (polyethylene glycol-block-polycaprolactone, or PEG-PCL) containing hyaluronic acid (HA) and Mn–Zn ferrite magnetic nanoparticles (MZF) were fabricated via a two-step preparation. HA-modified Mn–Zn ferrite magnetic nanoparticles (MZF-HA) can be enriched in CD44 highly expressing tumor cells, such as A549 (human lung adenocarcinoma cell line), through an active targeting mechanism via receptor–ligand binding of HA and CD44 (HA receptor). MZF can generate thermal energy under an AMF, leading to a local temperature increase to approximately 43 °C at tumor sites for mild HT, and the increased tumor oxygenation can enhance the therapeutic effect of RT. In vitro experiments show that MZF-HA is able to achieve excellent specific targeting performance toward A549 cells with excellent biocompatibility as well as enhanced therapy performance under HT and RT in vitro by apoptosis flow cytometry. In the A549 subcutaneous tumor xenografts model, MRI confirms the enrichment of MZF-HA in tumor, and hypoxia immunohistochemistry analysis (IHC) proved the increased tumor oxygenation after HT. Furthermore, the tumor volume decreases to 49.6% through the combination of HT and RT in comparison with the 58.8% increase of the untreated group. These results suggest that the application of MZF-HA is able to increase the therapeutic effect of RT on A549 and can be used for further clinical NSCLC treatment evaluation.
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CHEMOSPHERE
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2021
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IF 7.086
Han Qiao,Xiaoxiang Wang,Peng Liao,Cheng Zhang,Chongxuan Liu
A novel Mn(II) encapsulated mesoporous silica nanoparticles (Mn-MSNs) was developed for efficiently removing antibiotic tetracycline from aqueous solutions. The material has a well-ordered, hexagonal mesopore structure with a large specific surface area (720 m 2 /g) and maximum sorption capacity (229 mg/g) that is about an order of magnitude higher than that of mesoporous silica nanoparticles without Mn-encapsulated, or encapsulated with other transition metal cations Fe 3+ and Cu 2+ . Sorption results showed that the materials can sequestrate tetracycline within a large concentration range (5 μg/L–450 mg/L). Batch sorption experiment, spectroscopic analysis and density functional theory calculation collectively indicated that Mn–O complexation was the dominant mechanism for the tetracycline sorption. Electrostatic attraction and cation-π interaction also contributed to tetracycline sorption with their contribution levels varying with pH in a synergetic way with the Mn–O complexation. The Mn(II) encapsulated MSNs exhibited a good regeneration property over five repeated sorption-desorption cycles, demonstrating its promising potential in the cost-effective applications of sequestrating tetracycline from wastewater, drinking water , and contaminated solutions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Runren Jiang,Guanghua Lu,Min Wang,Tianjian Dang,Jianchao Liu,Zhenhua Yan
Utilizing photocatalysis to degrade pollution is emerging as a promising way to treat wastewater, but is challenged by low efficiency and scanty toxicity cognition. In this work, Mn 3 O 4 /BiOCl based crystal plane engineering systems are applied for naproxen (NPX) degradation, and Mn 3 O 4 /BiOCl 010 displayed better degradation rate, which is 16 and 8 times than that of the Mn 3 O 4 /BiOCl 001 and BiOCl 010 . According to the degradation pathway analysis and biological toxicity experiments, the toxicity of the degradation solution increased first and then decreased, which may be caused by the mineralization of NPX and more toxic intermediates. Affected by the distinct internal charge transfer directions of the two crystal planes of BiOCl, Mn 3 O 4 /BiOCl 010 heterojunction system has a faster charge transform than that of Mn 3 O 4 /BiOCl 001 . Moreover, the valence cycle of Mn can further accelerate the charge transfer, which can also provide a powerful driving force for NPX elimination.
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CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Jing Su,Tao Lyu,Hao Yi,Lei Bi,Gang Pan
A major challenge for effective decontamination of arsenate from aqueous solution is the development of adsorbent possessing enormous high-active sites with strong affinity to realize both high adsorption capacity and reduction of arsenate down to permissive levels. Here we demonstrate that this challenge may be overcome by doping Mn atoms into La 2 O 2 CO 3 materials. The synthesized material (5.26%-MnL) achieved an arsenate capture ability superior to most other currently-reported adsorbents, with the maximum adsorption capacity of 555.6 mg/g. Additionally, this novel adsorbent could dramatically reduce the concentration of arsenate from 3775 μg/L to less than 4 μg/L, well below the acceptable value for drinking water (10 μg/L). The adsorption capacity of 5.26%-MnL was demonstrated to be >300 mg/g over a wide pH range from 4 to 9 and the efficiency was maintained >85% even after three cycles of adsorption/desorption. Through a series of characterizations, both surface complexation and ion exchange were proved to contribute to arsenate removal at low molar ratios of As(V)/5.26%-MnL while forming LaAsO 4 precipitation played a greater role at higher As(V)/5.26%-MnL ratios. Density Functional Theory (DFT) calculations suggested that Mn atoms acted as active species by not only increasing lattice defects and adsorption sites, but also by activating La 3+ in La 2 O 2 CO 3 , which lowered the adsorption energy and facilitated arsenate removal. Due to the high affinity and superior adsorption capacity towards arsenate, Mn-doped La 2 O 2 CO 3 has been demonstrated to be a promising prospect for the remediation of arsenate-polluted water.
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NANOTECHNOLOGY
·
2019
·Vol. 31
·期 6
·065603
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IF 3.399
Chun Sun,Le Wang,Sijing Su,Zhiyuan Gao,Hua Wu,Zi-hui Zhang,Wengang Bi
White light-emitting diodes (WLEDs) based on all-inorganic perovskite CsPbX3 (X = Cl, Br, I) quantum dots (QDs) have attracted much attention and rely on mixing several colors of perovskites. However, this inevitably leads to a non-uniform light distribution and serious light loss. Here, a novel strategy was demonstrated to obtain white emission by combining the orange and blue emission from CsPb/Mn(Cl/Br)3 QDs. Notably, highly efficient white emission with a photoluminescence quantum yield of 94% was achieved by an anion exchange surface engineering (AESE) strategy. After AESE treatment the surface traps can be eliminated, resulting in improved exciton and Mn2+ emission. A prototype WLED device was fabricated and exhibited excellent optical stability, demonstrating great potential for perovskite QDs in the field of optoelectronics.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yuxiang Sun,Caiyun Yan,Jun Xie,Dan Yan,Ke Hu,Shengxin Huang,Jianping Liu,Yu Zhang,Ning Gu,Fei Xiong
Previous reports from our team revealed the significant potential advantage of Mn–Zn ferrite nanoparticles (NPs) in magnetic resonance imaging (MRI), whereas anisotropic NPs reportedly increased the blood circulation time of nanocarriers. Thus, anisotropic Mn–Zn ferrite displayed a huge potential in cancer synchronous diagnosis and treatment, that is, enhanced MRI observation was performed simultaneously when drug-targeted delivery therapy was applied to the tumor. Here, we developed three shaped Mn–Zn ferrite (Mn0.63Zn0.37Fe2O4) MNPs used as cancer theranostic nanoagents and compared the effect of the three shaped MNPs on cancer theranostics. Compared to the monodisperse sphere MNPs (S-MNPs-PPR) and clustering MNPs (C-MNPs-PPR), worm-like Mn–Zn ferrite MNPs (W-MNPs-PPR) achieved better results in T2-weighted MRI and achieved more sustained drug release than S-MNPs-PPR and more complete drug release than C-MNPs-PPR in vitro. Additionally, polyethylene glycol (PEG) coating and RGD modification encouraged the three shaped MNPs to evade the recruitment of macrophages more easily and to target the integrin-enriched endothelial cells instead. Meanwhile, W-MNPs-PPR coupled with Paclitaxel (PTX) exhibited more delivery of PTX in the integrin-enriched cells than the other two shaped MNPs, and the content of PTX was far more than that of the wild-type Taxol control group. What is more, in vivo results demonstrated that PTX-coated W-MNPs-PPR not only gained good dual-mode imaging in the tumor (MRI and fluorescence images) but also achieved longer blood circulation time and more PTX-targeted delivery to the tumor, as well as more efficiency in tumor cell killing, which make the simultaneous diagnosis and treatment of tumors to be conducted. Therefore, our works further revealed the importance of the NP shape on its functionality and ultimately provided an alternative and efficient worm-like theranostic nanoagent for tumor theranostics.
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IONICS
·
2019
·Vol. 25
·期 11
·5485-5494
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IF 2.289
Wang Xiaoqing,Tian Songran,Zhang Xiaoqing,Li Guoyan,Liu Ying,Chen Botao,Cheng Bowen
A 3D Ni 3 S 2 @Mn-Co-OH/NF cross-linked nanosheet heterostructure composite electrode has been successfully fabricated by a facile two-step hydrothermal method. The as-prepared Ni 3 S 2 @Mn-Co-OH/NF composite electrode exhibits a high capacitance (3163 F g −1 at a current density of 3 mA cm −2 ), a superior rate performance (2071 F g −1 at a current rate of 30 mA cm −2 ), and stable cycling property (maintaining 96.6% of the initial capacitance after 4000 cycles at a current rate of 10 mA cm −2 ). This excellent electrochemical performance can be ascribed to the unique cross-linked nanosheet heterostructure formed directly on Ni foam current collector and the synergistic effect between Mn-Co-OH and Ni 3 S 2 of the composite electrode.
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ACS Applied Materials & Interfaces
·
2018
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IF 8.097
Weiwei Chen,Tongchao Shi,Juan Du,Zhigang Zang,Zhiqiang Yao,Meng Li,Kuan Sun,Wei Hu,Yuxin Leng,Xiaosheng Tang
As an outstanding less-Pb candidate, doping Mn2+ ions into perovskite quantum dots (QDs) has received significant interest in the application of light-emitting diodes (LEDs). However, their further applications are impeded by poor chemical instability. Here, the silica-wrapped Mn-doped CsPbCl3 QDs are fabricated via hydrolyzing (3-aminopropyl) triethoxysilane with improved operational stability. Also, the photoluminescence quantum yield as high as 55.4% for the CsPbMnCl3@SiO2 composite is achieved. Silica wrapping can protect the perovskite QDs from damage by temperature and humidity as well as anion exchange. Furthermore, white LED devices are prepared by employing the mixture of green CsPbBr3 QDs and orange-red CsPbMnCl3@SiO2 composites. The as-obtained white LED device operated at a forward current of 20 mA exhibits bright natural light with a high luminous efficiency of 77.59 lm/W, and the corresponding color rendering index of 82 and color temperature (CCT) of 3950 K are obtained. Additionally, the electroluminescence spectrum shows nearly no variation after 24 h operation. This work will promote the Mn-doped CsPbCl3 QDs material to the practical application in solid-state LEDs.
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