JOURNAL OF HAZARDOUS MATERIALS
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2025
·
IF 11.3
Hong Meng,Junhui Zhou,Chunyang Nie,Wenhao Li,Didi Li,Yongqing Zhang,Zhimin Ao
Understanding the metal bonding types in biochar and their effects on peroxymonosulfate (PMS) activation is essential for selecting appropriate biomass and developing efficient catalysts. This study reports a dual-pathway non-radical oxidation system activated by Mn-doped biochar (P-Mn-TPs-900). In the P-Mn-TPs-900/PMS system, phenol degradation reached 100 % within 60 min across a broad pH range (5 −10). Additionally, this oxidation system exhibited excellent stability (5 cycles), maintaining at least 74 % degradation efficiency in the presence of background ions or humic acid. Experimental results and density functional theory (DFT) calculations identified: i) C-O-Mn sites as the primary active sites for PMS activation, facilitating the formation of singlet oxygen ( 1 O 2 ) which was the key reactive oxygen species for phenol degradation; ii) phenol adsorbed on the P-Mn-TPs-900 surface was degraded via an electron transfer process between sulfate groups and phenol. DFT calculations showed strong hybridization between the Mn 3d-orbital, the O 2p-orbital, and the corresponding 2p-orbitals of carbon, which enhanced biochar's catalytic capability. This study provides insights into the role of the C-O-Mn site in PMS activation and offers guidance for selecting suitable biomass for developing practical Fenton-like systems in wastewater treatment.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Zhaowu Wang,Zhiyu Min,Liping Tian,Wenrui Zhang,Hao Li,Jinlong Chen,Derong Zhu
Mn⁴⁺-activated fluoride bulk crystals have recently emerged as promising phosphor materials due to their superior water resistance, thermal stability, and quantum efficiency compared to conventional powder forms. Herein, we report the successful growth of millimeter-sized (NH₄)₂SiF₆:Mn⁴⁺ crystals with intense red emission under 365 nm UV excitation via a facile cooling crystallization approach. The as-grown crystals exhibit a distinctive yellow body color and attain dimensions of up to ∼3 mm. Intriguingly, Mn⁴⁺-doping triggers a structural phase transition in the host matrix from cubic symmetry (space group, Fm- 3 m ) to hexagonal symmetry (space group, P 6 3 mc ), accompanied by progressive lattice distortions. This structural evolution manifests spectroscopically through the emergence of a zero-phonon line (ZPL) in photoluminescence spectra, with the ZPL-to- v ₆ intensity ratio escalating from 0 % to 34 % as Mn⁴⁺ concentration increases. Concomitantly, all seven characteristic emission peaks display systematic blueshifts. Furthermore, the microscopic morphology, thermal quenching behavior, and decay property of the crystal are significantly influenced by the doping-induced structural modifications. This study establishes a structural engineering strategy for optimizing luminescent performance in (NH₄)₂SiF₆:Mn⁴⁺ crystal phosphors.
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CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 12.5
Chao Liu,Chaojie Wang,Bingxu Chen,Haitao Lu,Wei Ding,Hong Li
Conventional manganese(II) (Mn(II))-activated sulfite (S(IV)) systems remain constrained by slow reaction kinetics and inefficient Mn redox cycling, limiting their application in water treatment. Although non-radical pathways have been reported in certain metal/S(IV) systems, the role of high-valent Mn species remains unresolved. To address this knowledge gap, this study engineered a Mn-based metal-organic framework (Mn-MOF, denoted MM) featuring unsaturated Mn(II)−OH sites to achieve efficient S(IV) activation and redirect the oxidation process toward a non-radical route. Arsenite (As(III)) was employed as a model contaminant to systematically evaluate the MM/S(IV) system through kinetic analysis, reactive species identification, and surface characterization. The MM/S(IV) system enabled rapid As(III) oxidation (99.3% within 5 min, 0.64 min −1 ) at pH 7.4. The catalyst exhibited excellent stability during sequential operation (0.04% Mn leaching) and could be nearly fully regenerated. Mechanistic investigation revealed an interfacial pathway initiated by an O 2 -assisted, ligand-bridged electron transfer that yielded SO 3 •− /SO 5 •− . SO 5 •− subsequently oxidized Mn(II) to Mn(III), which then underwent two-electron oxidation by HSO 5 − to form Mn(V) as the dominant oxidant. This work demonstrates how MOF coordination engineering can redirect S(IV) activation toward a non-radical Mn(V)-mediated route, advancing the design of metal-centered oxidation systems for water remediation.
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Chemical Science
·
2024
·Vol. 15
·期 5
·1894-1905
·
IF 7.6
Chengyu Zhang,Xiangyang Wang,Renyuan Zhao,Fabrice Ndayisenga,Zhisheng Yu
Tuning the electron distribution of metal single-atom active sites via bimetallic clusters is an effective way to enhance their hydrogen evolution reaction (HER) activity, but remains a great challenge. A biochar-based electrocatalyst (BCMoMn800-2) with both MnN4 active sites and Mo2C/Mn7C3 clusters was synthesized using in situ enriched Mo/Mn biomass as a precursor to trigger the HER. Various characterization and density functional theory (DFT) calculation results indicated that the presence of Mo2C/Mn7C3 clusters in BCMoMn800-2 effectively induced the redistribution of charges at MnN4 sites, reducing the energy of H* activation during the HER. In 0.5 M H2SO4, the overpotential was 27.4 mV at a current density of 10 mA cm−2 and the Tafel slope was 31 mV dec−1, and its electrocatalytic performance was close to that of Pt/C. The electrocatalyst also exhibited excellent electrocatalytic stability and durability. This work might provide a new strategy for solid waste recycling and constructing efficient HER electrocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Ke Li,Yibing Sun,Jiawei Zhou,Xinyue Zhang,Hongchao Li,Zhichao Yang
The combination of transition metal oxides with carbon-based materials is a promising strategy for constructing efficient catalysts for peroxymonosulfate (PMS) activation to degrade aqueous organic contaminants. However, the complex heterostructure of the composites often hinders the identification of the actual reactive species responsible for pollutant degradation. In this study, we integrate Mn 3 O 4 into N-doped graphite (NG) to elucidate the mechanisms involved in the Mn-NG composite mediated PMS activation process. The Mn-NG/PMS system shows excellent performance in oxidizing bisphenol A (BPA) over a wide pH range (3.4 to 9.4) and in the presence of co-existing substrates. Mn sites in Mn 3 O 4 are responsible for the activation of PMS, and the NG matrix enhances the dispersion of Mn in the Mn-NG composite. Multiple experimental results indicate that free radicals (i.e., hydroxyl radicals (HO • ) and sulfate radicals (SO 4 •− )) are not generated, and surface reactive Mn(IV) is proposed as the primary reactive species for BPA oxidation. This study provides new insights into understanding the role of Mn oxides in carbon-based composites in PMS activation for degradation of organic pollutants.
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CATALYSIS LETTERS
·
2017
·Vol. 148
·期 1
·181-193
·
IF 2.799
Lin Jin,Guo Yafei,Chen Xiao,Li Changhai,Lu Shouxiang,Liew Kim Meow
Abstract Nanostructured CeO 2 supported CuO–MnO 2 (CuMn/Ce) catalysts were synthesized by wet co-impregnation method and compared with CuO/CeO 2 and MnO 2 /CeO 2 catalysts on CO oxidation. The former shows significantly higher catalytic activity toward CO oxidation than the bimetallic oxides catalysts with minimum T 50 . Dual synergistic effects in the interfaces of CuO–MnO 2 and CuO–CeO 2 shall be responsible for the higher oxidation performance of CuMn/Ce catalyst. As Cu/Mn mass ratio varies from 1/0.2 to 1/9, CO oxidation activities of the catalysts present unimodal distribution, and the catalyst with Cu/Mn = 1/1 shows the highest performance (T 50 = 45.8 °C; Ea = 24.11 kJ mol −1 ). Cu acts as CO dissociative adsorption sites, and Mn–Ce supplies activated O species from gas molecule and lattice oxygen, which are both indispensable for improving utilization efficiency of the reactants in the dual redox processes. The catalytic performance of catalyst is also vitally correlated with calcination temperature (160–320 °C). The optimum calcination temperature of CuMn/Ce catalyst is 320 °C. Catalyst characterization results indicate that the pretreatment at 320 °C is decent to obtain desired metal oxides along with fine texture properties. Graphical Abstract
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NANO LETTERS
·
2022
·
IF 12.262
Jia-Min Lai,Muhammad Umair Farooq,Yu-Jia Sun,Ping-Heng Tan,Jun Zhang
The multiphonon process plays an essential role in understanding electron–phonon coupling, which significantly influences the optical and transport properties of solids. Multiphonon processes have been observed in many materials, but how to distinguish them directly by their spectral characteristics remains controversial. Here, we report high-order Raman scattering up to 10 orders and hot luminescence involving 11 orders of phonons in Mn-doped ZnO nanowires by selecting the excitation energy. Our results show that the intensity distribution of high-order Raman scattering obeys an exponential decrease as the order number increases, while hot luminescence is fitted with a Poisson distribution with a resonance factor. Their linewidth and frequency can be well explained by two different transition models. Our work provides a paradigm for understanding the multiphonon-involved decay process of an excited state and may inspire studies of the statistical characteristics of excited state decay.
研究领域:
凝聚态物理
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材料科学
·
光谱学
·
纳米材料
·
固体物理
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Kai Li,Shengjun Xu,Xiaobiao Liu,Huiji Li,Sihui Zhan,Shuanglong Ma,Yan Huang,Shiliang Liu,Xuliang Zhuang
A family of graphene-based activators including reduced graphene oxide (RGO), nitrogen doped reduced graphene oxide (NRGO), zero-valent manganese loaded reduced graphene oxide (Mn-RGO) and zero-valent manganese loaded N-doped reduced graphene oxide (Mn-NRGO) were fabricated to activate peroxymonosulfate (PMS) for bisphenol A (BPA) degradation. A significant synergistic effect between loaded manganese nano-particles (Mn-NPs) and doped N was revealed by comparing the apparent reaction rate constants with about 12.4, 7.6 and 10.5-folds enhancement when compared Mn-NRGO with RGO, NRGO, Mn-RGO, respectively. By integrating the results of chemical scavenger experiment, electron paramagnetic resonance test, galvanic oxidation process, PMS stoichiometric efficiency, linear sweep voltammetry and in-situ Raman spectrum, a predominant outer-sphere catalyst-PMS complexes mediated electron transfer pathway was uncovered. Based on kinetic studies, the specific contribution of synergistic effect was quantified to be at least 70%. The calculated Fermi level advanced by 0.03 eV in Mn-NG compared with that in NG, demonstrating that Mn-NG is more liable to donate electrons to PMS. The E ads and l O-O results pointed out that synergistic effect between Mn-NPs and doped N relied on the intimate affinity between Mn-NPs and HSO 5 – which triggered more uneven distribution of charge on the whole carbon sheets, and more adsorption of HSO 5 – on carbon framework. These newly created adsorption consequently reinforcing the formation of catalyst-PMS complexes and the elevation of mediated electron transfer pathway. Overall, this study firstly provides a comprehensive and definite insight of the synergistic effect between loaded Mn-NPs and doped-N on carbon materials for promoting PMS activation to degrade organics.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Xiaodan Zhang,Ai Yuan,Xuanxiang Mao,Qiumeng Chen,Yuming Huang
We report that the Co/Mn oxides nanocomposite, obtained by directly pyrolying cobalt doped Mn-BTC precursor, is a new oxidase mimetic for colorimetric sensing of acid phosphatase (ACP). By tuning the molar ratios of cobalt ions to Mn-BTC (BTC = 1,3,5-benzenetricarboxylate) precursor, four bimetal Co/Mn-BTCs and their derivatives were obtained. These Co/Mn oxides showed 1.4-fold to 2.6-fold higher oxidase-like activity than that of Mn 2 O 3 derived from Mn-BTC, indicating that Co-doping is an effective way for improving and tuning oxidase-like activity of manganese oxides. The rambutan-like Co/Mn oxides with Co/Mn molar ratio of 0.33 (denoted CMO-0.33) in the MOFs precursors exhibited the highest oxidase-like activity. The estimated Michaelis constant for 3,3′,5,5′-tetramethylbenzidine (TMB) was 2.26-fold lower than that of Mn 2 O 3 , indicating its stronger affinity to TMB. Based on the inhibitory effect of ascorbic acid (AA) on the TMB-CMO-0.33 system, a new colorimetric strategy was paved for screening ACP activity when coupled with L-ascorbic acid 2-phosphate trisodium salt (AAP) because ACP could catalyze hydrolysis of AAP to generate AA. The proposed colorimetric biosensor allows detection of ACP in the range 0.02–1.0 U/L with a limit of detection of 8.2 mU/L. Its potential utilization in ACP assay in human serum samples is successfully demonstrated.
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JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Wei Wang,Mengrui Li,Liang Liu,Xiaoshuang Zhou,Xiankai Li,Kewei Zhang,Lina Chen,Jun Wei,Long Chen
To meet the practical demands of flexible fiber-shaped supercapacitors (FSSCs) for wearable electronics, it's crucial to develop electrodes with both high energy density and flexibility. In this work, an ultrahigh capacitance (Co,Mn)(Co,Mn) 2 O 4 /Ni(OH) 2 (CMO/Ni(OH) 2 ) fiber electrode is designed. The (Co,Mn)(Co,Mn) 2 O 4 (CMO) nanosheets possessing large specific surface area and enriched active sites, which can be served as nano-substrate for the electrodeposition of Ni(OH) 2 . This special structure facilitates the exposure of more electroactive sites and accelerate rapid electrons transfer, resulting in boosted electrochemical performance. Benefiting from these advantages, the area capacitance of the CMO/Ni(OH) 2 electrode is up to 4787.6 mF cm −2 at 1 mA cm −2 , which is approximately 15 times higher than that of the CMO (311 mF cm −2 ), and 6.7 times higher than that of the Ni(OH) 2 (718 mF cm −2 ). Coupled with activated carbon (AC) electrode, the assembled all-solid-state CMO/Ni(OH) 2 //AC FSSCs demonstrate a high energy density of 89.45 μW h cm −2 at 1505 μW cm −2 , along with great flexibility and stability. Moreover, these devices can be integrated into clothes, and electronic watch, serving as an energy supply. This work offers a novel approach to designing high-performance fiber electrode for wearable flexible energy storage devices.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shaozhi Liu,Honggang Zhang,Guangyao Zhai,Zeyan Wang,Hefeng Cheng,Peng Wang,Zhaoke Zheng,Ying Dai,Baibiao Huang,Yuanyuan Liu
Ozonation assisted photocatalytic (OPC) nitrogen oxidation provides a new sustainable strategy for nitrate production, yet the inefficient activation of N 2 and the rapid recombination of photogenerated carrier remains a challenge. Herein, the BiOBr-based catalysts with Mn single atoms and oxygen vacancies is designed for the OPC N 2 oxidation. Under optimal conditions, the yield of NO 3 − over Mn 0.035 /O v -BiOBr is as high as 151.3 μmol g −1 h −1 , which are 7.63 times that over BiOBr (19.8 μmol g −1 h −1 ). Detailed experimental analysis reveals a synergistic effect between Mn single atoms and oxygen vacancies, where Mn single atoms act the active site for N 2 adsorption and reaction, and oxygen vacancies for O 3 activation and transformation. Theoretical calculations further demonstrate that the synergistic effect between Mn single atoms and oxygen vacancies not only enhance the dipole moment along the [001] direction (i.e. the interlayers), but also induce a dipole moment within the [Bi 2 O 2 ] 2+ layer, both of which are advantageous for chare separation and the subsequent transformation of O 3 to reactive oxygen species (ROS). Meanwhile, a variety of active species act cooperatively to sped up the N 2 oxidation process. This work provides a new method for efficient N 2 oxidation to NO 3 − , namely photocatalytic ozonation, and also provides a deep understanding for the modulation of the internal electric field (IEF) effect of BiOBr via both single atoms and oxygen vacancies to improve charge separation.
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WATER RESEARCH
·
2026
·
IF 12.8
Tianming Zheng,Peifang Wang,Bin Hu,Chongchong Liu,Ruoxi Zhen
Aquaculture activities discharge large amounts of antibiotics, with protein-like dissolved organic matter (DOM) coexisting in wastewater, whose impact on FF degradation remains unclear. An efficient advanced oxidation process (AOP) was established by Mn(II), nitrilotriacetic acid (NTA), and peroxymonosulfate (PMS) for degrading the typical aquaculture antibiotic florfenicol (FF), achieving removal efficiency of (97.38±1.02)% within 20 min primarily via Mn(V)= O , in which •OH, •SO 4 - , and 1 O 2 made minor contributions. The inhibitory effects of fishery amino acids on FF degradation followed the order: poly lysine > tryptophan > methionine > lysine. Based on electrochemical measurements and density functional theory (DFT) calculations, tryptophan and methionine competed for PMS binding sites, with methionine being preferentially oxidized by Mn(V)= O , thereby delaying FF degradation. Primary degradation pathways involved defluorination, dechlorination, and aromatic ring hydroxylation, exhibiting a reduced toxicity. Overall, this study developed a sustainable strategy to remove typical fishery antibiotics, highlighting the critical role of Mn(V)= O and the interference mechanism of protein-like DOM.
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