ACS Catalysis
·
2026
·Vol. 16
·期 17
·17380-17391
·
IF 13.6
Ma Meifeng,Zhang Rongwang,Deng Shaorong,Zhao Xilai,Yang Fei,Fang Xiuzhong,Wang Xiang,Xu Xianglan
Rational design of highly active catalysts for low-temperature CO 2 methanation remains a critical challenge for efficient CO 2 utilization. Herein, we demonstrate that Mn incorporation into the Cr 2 O 3 lattice, rather than surface modification, markedly enhances the catalytic performance of Ru/Cr 2 O 3 catalysts. The optimal Ru/Mn 0.10 Cr 0.90 O x catalyst (2.24 wt % Ru) achieves 91% CO 2 conversion at 200 ° C with a space velocity of 36,000 mL g cat –1 h –1 , substantially exceeding that of the parent Ru/Cr 2 O 3 (4% at 200 ° C). Compared with Ru/Cr 2 O 3 , Ru/Mn 0.10 Cr 0.90 O x exhibits a 4.1-fold higher turnover frequency at 180 ° C, confirming the intrinsic catalytic enhancement conferred by Mn lattice doping. Comprehensive characterization revealed that Mn lattice doping generates Mn-O-Cr bonds, creating distinct Ru/O-Cr-O v -Mn interfacial sites in contrast to the Ru/O-Cr-O v -Cr interfaces present in undoped Ru/Cr 2 O 3 . In situ DRIFTS and H 2 -TPSR-MS studies demonstrated that low-temperature CO 2 methanation on Ru/Mn 0.10 Cr 0.90 O x proceeds concurrently via both CO* and HCOO* intermediate pathways, whereas only the CO* pathway operates on Ru/Cr 2 O 3 . DFT calculations revealed that Mn doping selectively modulates CO 2 adsorption at the interface while minimally affecting bridged Ru sites. At the Ru/O-Cr-O v -Mn interface, oxygen vacancies form and regenerate more readily than at the Ru/O-Cr-O v -Cr interface during CO 2 methanation, enabling an additional HCOO* pathway. This dual-pathway mechanism fundamentally underpins the enhanced low-temperature activity of Ru/Mn 0.10 Cr 0.90 O x and provides a promising design strategy for developing efficient CO 2 methanation catalysts.
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Frontiers in Chemistry
·
2023
·
IF 5.5
Sun Lixia,Hu Jiayan,Bai Weiqi,Mao Wutao,Song Zhongcheng
The hunt for a higher power storage, relatively inexpensive, non-polluting battery technology is currently a pressing issue because of the rapid growth of the worldwide economic and the progressively significant environmental pollution. Among the possible nanomaterials for rechargeable batteries that can have heteroatoms applied to it in order to improve its electrochemical behavior is LixTiy(PO4)3. Carbon-coated Mn-doped Li2Mn0.1Ti1.9(PO4)3 materials was synthesized by spray drying method. The material was characterized by XRD, SEM, TEM, BET, TGA et al. Crystal data refinement results by Rietveld method showed that the symmetry space group is Pbcn.The lattice parameters of Li2Mn0.1Ti1.9(PO4)3 are a = 11.9372 Å, b = 8.5409 Å, c = 8.5979 Å, α = β = γ = 90°, V = 876.59 Å3 and Z = 4). Rietveld refinement was performed, and the confidence factors are Rwp = 11.79%, Rp = 9.14%, and χ2 = 1.425. It was exhibited that LMTP0.1/CA-700 material has good crystallinity. Testing the cells with LAND test procedure (200 mA/g current density for 200 cycles), the LMTP0.1/CA-700 material has a discharge specific capacity of about 65 mAh/g. The capacity decayed by only 3% during the cycle. It has some potential application values as cathode of lithium ion battery in the future.
研究领域:
材料科学
·
电化学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 25
·38006-38016
·
IF 5.19
Wang Luyao,Wang Hanlin,Liu Haibo,Zou Xuehua,Chen Dong,Chu Ziyang,Hu Jinchao,Chen Tianhu
Naturally occurring Mn-rich limonite mainly composed of goethite and manganese oxides was used to remove tetracycline (TC) from the aqueous solution. The effects of dosage, initial solution pH, temperature, and coexisting anions on TC removal were investigated. Results showed that 95% of TC (30.0 mg·L −1 ) was removed in a wide pH range of 3.0–9.0 by limonite with high specific surface area (145.0 m 2 ·g −1 ) and mesoporous structure. The presence of Cl − , NO 3 − , and SO 4 2− in the studied concentration range did not influence TC removal efficiency significantly, while PO 4 3− inhibited the adsorption of TC over limonite due to the competition with TC for active sites. Integrated with the FT-IR analysis, electrostatic interaction and complexation were proved to be the adsorption mechanisms of TC by limonite. The quenching experiments and ESR analysis revealed that singlet oxygen ( 1 O 2 ) also was involved in TC degradation. In addition, limonite displayed an efficient recycling performance and stability after four cycles. This study revealed that the Mn-rich limonite was a promising adsorbent for TC removal from aqueous solutions and promoted the application of natural mineral material in the environmental field.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8611-8618
·
IF 3.925
Jing Huang,Qi Shan,Yanan Fang,Ning Zhao,Xiaomiao Feng
A new simple strategy to prepare Mn–Fe Prussian blue analogue (PBA) derived oxide micromotors through co-precipitation and heat treatment is demonstrated. The morphology of the precursors could be precisely controlled from cubic-like to spherical-like by introducing citrate. Because of the synergistic catalytic reaction of bimetallic Mn–Fe oxides, micromotors with different shapes could be powered efficiently in H2O2 solution. In particular, the obtained cubic Mn–Fe oxide micromotors showed strong propulsion at a speed of 71.21 μm s−1 in 1% H2O2 solution. With dual mechanisms of adsorption bubble separation (ABS) and Fenton oxidation, the cubic Mn–Fe oxide micromotors showed extraordinary removal ability for Rhodamine B (RhB) as a simulated pollutant and could remove up to 95.2% of RhB within 30 minutes. Magnetic Fe3O4 contained in the component not only could degrade organic pollutants, but also could be recycled by magnetic field and reused with high degradation efficiency. These dual-functional metal oxide catalytic micromotors provide a practical and environmentally friendly strategy for environmental restoration.
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JOURNAL OF CHEMICAL CRYSTALLOGRAPHY
·
2022
·Vol. 53
·期 1
·145-151
·
IF 0.582
Zhang Lirong,Qi Feiyan,Shele Muge,Namila E.,Qi Liming,Baiyin Menghe
One quaternary selenidoantimonate of [Mn(en) 3 ]CdSb 2 Se 5 ( 1 ) (en = ethylenediamine) was prepared under 1,2-propanediamine condition by mild solvothermal method. Single-crystal X-ray diffraction analysis reveals that compound 1 crystallizes in the monoclinic space group C 2/c. Its structure consists of infinite 1D [CdSb 2 Se 5 ] n 2n− anionic chains and [Mn(en) 3 ] 2+ cations. Meanwhile, “Z” shaped eight-membered [Cd 2 Sb 2 Se 4 ] and six-membered [CdSb 2 Se 3 ] rings are alternately found. As estimated from UV–Vis absorption spectrum, the band gap of 1 is 2.58 eV. Compound 1 also showed rapid response and excellent reproducibility based on photoelectric test. In addition, the magnetic and other properties of 1 were studied. Graphical Abstract The manuscript describes the synthesis, crystal structure, single-crystal X-ray diffraction, elemental analysis, photoelectric response, thermogravimetric analysis, magnetic properties, infrared spectroscopy and UV-Vis diffuse reflectance spectroscopy of [Mn(en) 3 ]CdSb 2 Se 5 . The photoelectric response of compound 1 was explored, and a highly repetitive and stable photocurrent curve was found, indicating that 1 is a typical p-type semiconductor. In addition, the magnetism of compound 1 was also studied, which showed that 1 had antiferromagnetic behavior.
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 39
·期 10
·2685-2690
·
IF 3.146
Wu Kang,Zhang Zhongliang,Hua Fei,Ye Zhou,Li Chao,Yao Youzhi
Sewage containing antibiotics is harmful to the water environment. Here, a newly prepared iron manganese binary oxide (FMBO) activated persulfate (PDS) has excellent performance for the degradation of sulfapyridine (SPY) in an aqueous environment. The effects of initial pH, SPY, PDS concentration and FMBO dosage on the degradation ability of SPY were investigated. When the pH of FMBO/PDS was 4.0 and the initial concentration of PDS was 2.0 mmol/L, the degradation ratio of SPY could reach 94.4%. In the system of removing organic pollutants by transition metal activated PDS, SO
−• 4
and •OH radicals are generally generated, and •OH radical plays a major role. Through the identification of SPY intermediate products by LC/MS, the degradation mechanism was explored. The degradation pathway showed that the strong oxidation of FMBO and the activity of PDS promoted the production of hydroxyl radical and contributed to the degradation and transformation of antibiotics. This study shows that FMBO/PDS has high degradation efficiency in the degradation of SPY.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 46
·期 2
·490-497
·
IF 3.591
Shaoju Jian,Yiting Cheng,Xiaofan Ma,Hongtao Guo,Jiapeng Hu,Kaiyin Zhang,Shaohua Jiang,Weisen Yang,Gaigai Duan
La–Mn bimetal oxide nanofibers, used as an adsorbent for the defluoridation of water, were synthesized by an electrospinning and heat treatment technology. The La–Mn bimetal oxide nanofiber adsorbent with a specific surface area of 35.064 m2 g−1 displayed a good defluoridation performance. Both the adsorption kinetics and equilibrium for fluoride (F−) uptake onto La–Mn bimetal oxide nanofibers were investigated. The kinetic studies established that the adsorption attained equilibrium at about 90 min, and the PSO kinetic model was ideal for the kinetic data under 20 and 50 mg L−1. The Langmuir maximum F− uptake was computed to be 189.39 mg g−1 at 308 K and pH 3. A thermodynamic study affirmed a feasible, endothermic, spontaneous and entropy driven process of F− adsorption towards La–Mn bimetal oxide nanofibers at the studied temperature range. Except for the competitive adsorption of PO43− and F−, the presence of NO3−, CO32−, Cl− and SO42− had little effect on fluoride removal. The La–Mn bimetal oxide adsorbent exhibited a good reusability.
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INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Jianping Zhao,Fei Qian,Wenping Guo,Jianfeng Li,Zeyuan Lin
Three different manganese(II) porphyrins have been exploited to react with 4-methylimidazolate (4-MeIm–), and the five-coordinate products are characterized by ultraviolet–visible, single-crystal X-ray, and electronic paramagnetic resonance spectroscopies. Interestingly, 4-MeIm– is found to bond to the metal center through either of the two N atoms (N1 or N3), which yielded two linkage isomers with either an unhindered or a hindered ligand conformation, respectively. Investigations revealed it is the large metal out-of-plane displacements (Δ24 and Δ4 ≥ 0.59 Å) that have rendered the equivalence of two isomers with a small energy difference (5.2–8.3 kJ/mol). The nonbonded intra- and intermolecular interactions thus become crucial factors in the balance of linkage isomerization. All of the products in both solution and solid states show the same characteristic resonances of high-spin Mn(II) (S = 5/2) with g⊥ ≈ 5.9 and g∥ ≈ 2.0 at 4 K, consistent with the weak effects of the axial ligand on core conformation and metal electronic configurations. Zero-field splitting parameters obtained through simulations are also reported.
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DRUG DELIVERY
·
2021
·
IF 6.419
Jiali Li,Xue Jiang,Lihuan Shang,Zhen Li,Conglian Yang,Yan Luo,Daoyu Hu,Yaqi Shen,Zhiping Zhang
This study aimed to synthesize and characterize L-epigallocatechin gallate (EGCG) complexed Mn2+ nanoparticle (L-EGCG-Mn), a proof-of-concept pH-sensitive manganese core nanoparticle (NP), and compare its magnetic resonance (MR) properties with those of Gd-DTPA, both in vitro and in vivo. Reverse microemulsion was used to obtain the L-EGCG-Mn NPs. The physicochemical properties of L-EGCG-Mn were characterized using dynamic light scattering, transmission electron microscopy, and near-infrared fluorescence small animal live imaging. The in vitro relaxivity of L-EGCG-Mn incubated with different pH buffer solutions (pH = 7.4, 6.8, 5.5) was evaluated. The T1-weighted MR imaging (MRI) properties were evaluated in vitro using hypoxic H22 cells as well as in H22 tumor-bearing mice. Cytotoxicity tests and histological analysis were performed to evaluate the safety of L-EGCG-Mn. L-EGCG-Mn showed good biocompatibility, stability, pH sensitivity, and tumor-targeting ability. Moreover, when the pH was decreased from 7.4 to 5.5, the r1 relaxivity of L-EGCG-Mn was shown to gradually increase from 1.79 to 6.43 mM−1·s−1. Furthermore, after incubation with L-EGCG-Mn for 4 h, the T1 relaxation time of hypoxic H22 cells was significantly lower than that of normoxic H22 cells (1788 ± 89 vs. 1982 ± 68 ms, p=.041). The in vivo analysis showed that after injection, L-EGCG-Mn exhibited a higher MRI signal compared to Gd-DTPA in H22 tumor-bearing mice (p < .05). Furthermore, L-EGCG-Mn was found to have a good safety profile via cytotoxicity tests and histological analysis. L-EGCG-Mn has a good safety profile and pH sensitivity and may thus serve as a potential MRI contrast agent.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2020
·
IF 3.99
Jiahui Deng,Yalin Cheng,Min Liu,Biyang Tu,Shan Xue,Haisheng Tao
In this study, Fe-Mn co-embed sodium alginate carbon spheres (Fe-Mn/SA-C) were prepared as a cost-effective adsorbent for aqueous Cd(II) removal by a facile pyrolysis method. The morphology and chemical composition of Fe-Mn/SA-C were explored with various characterized techniques. The results indicate that Fe-Mn/SA-C possess porous structures and abundant oxide-based functional groups. Fe-Mn/SA-C exhibits excellent adsorption properties for aqueous Cd(II) and the adsorption process is pH-dependent. The adsorption data could fit pseudo second-order and Langmuir models well, suggesting that chemisorption is a dominant adsorption mechanism and the maximum adsorption capacity is 280.11 mg −1 . Thermodynamic analysis demonstrates that the adsorption is spontaneous and endothermic. The adsorption mechanisms of Cd(II) include the complexation of Cd(II) with oxygen-based functional groups, precipitation, and ion exchange. Finally, the granulated and magnetic Fe-Mn/SA-C is an efficient and practical adsorbent for cadmium-containing wastewater treatment.
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OPTICAL MATERIALS
·
2020
·
IF 2.779
Yuqian Wang,Honghong Lei,Peng Jiang,Kunyang Cui,Lin Liu,Bin Li,Wenbin Cao
The solid solution of Ba 3 Al 2- x Mn x O 6+ y (0 ≤ x ≤ 0.2) is successfully synthesized through solid state reaction. The colors of compounds are tuned from sky blue ( x ≤ 0.1) to ocean blue ( x = 0.2) with the increase of Mn content. The X-ray diffraction data shows that the major phase of all the as-synthesized samples is cubic Ba 3 Al 2 O 6 structure with the space group of P 2 1 3. The oxidation state of Mn is confirmed to be +5 by X-ray photoelectron spectroscopy analysis. UV–Vis absorption spectroscopy demonstrates that the sample's color comes from the d - d transition of Mn 5+ located in [AlO 4 ].
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ACS Catalysis
·
2023
·
IF 12.9
Yanfen Fang,Dengyu Ying,Huibin Niu,Yan Xu,Shaobin Wang,Ran Duan,Huaiyong Zhu,Chaoyuan Deng,Chuncheng Chen,Yingping Huang
Although metal-rich biochar (M-BC) is widely used in soil remediation and pollution control, the activation mechanism of molecular oxygen (O2) by M-BC still needs to be clarified due to the low metal loading. In this study, we enhanced the manganese content of low-temperature manganese-rich biochar (Mn-BC) by treating it with hydrogen peroxide (H2O2), resulting in the formation of MnBC-Hx (where x represents the volume of H2O2 used in mL). MnBC-H5 was particularly effective in activating O2, leading to the successful degradation of phenol and dyes. Characterizations showed that the MnII in the outer layer of MnC2O4·2H2O nanoparticles evenly dispersed over Mn-BC was oxidized to MnIII by H2O2. This process was accompanied by the removal of coordinated H2O, resulting in the formation of MnIIIC2O4 on MnBC-H5. Under visible light irradiation, MnIII can bind to O2 to form MnIIIOOH species, which facilitates the transfer of charges and generates superoxide radicals (·O2–) that effectively degrade organics. Notably, MnIII of MnBC-H5 remains stable after the organic degradation reaction. This study will not only provide a theoretical basis for developing environmentally friendly biochar-based catalysts but also promote the study of the environmental effects of biochar.
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