Journal of the American Chemical Society
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2014
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IF 11.444
Jian Lin,Qian Zhang,Le Wang,Xiaochun Liu,Wenbo Yan,Tao Wu,Xianhui Bu,Pingyun Feng
We report a simple and yet effective method to introduce Mn2+ ions into semiconducting nanoclusters with atomically precise control. Our method utilizes one type of micrometer-sized crystals, composed of well-defined isolated supertetrahedral chalcogenide nanoclusters (∼2 nm, [Cd6In28S52(SH)4]) whose core metal site is unoccupied in as-synthesized pristine form. This unique model structure with vacant core site makes it possible to achieve ordered distribution of Mn2+ dopants, and at the same time effectively preclude the formation of Mn2+ clusters in the host matrix. A two-step synthesis strategy is applied to realize an atomically precise doping of Mn2+ ion into the core site of the nanoclusters, and to achieve uniform distribution of Mn2+ dopants in the crystal lattice. The PL, X-ray photoelectron (XPS), as well as the electron paramagnetic resonance (EPR) spectra reveal the successful incorporation of Mn2+ ion into the core site of the nanocluster. Different from the pristine host material with weak green emission (∼490 nm), the Mn2+-doped material shows a strong red emission (630 nm at room temperature and 654 nm at 30 K), which is significantly red-shifted relative to the orange emission (∼585 nm) observed in traditional Mn2+-doped II–VI semiconductors. Various experiments including extensive synthetic variations and PL dynamics have been performed to probe the mechanistic aspects of synthesis process and resultant unusual structural and PL properties. The quaternary semiconductor material reported here extends the emission window of Mn2+-doped II–VI semiconductor from yellow-orange to red, opening up new opportunities in applications involving photonic devices and bioimaging.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2017
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IF 3.133
Qiqi Nie,Yongbo Wang,Licong Jia,Bei Liu,Enzhou Liu,Xiaoyun Hu,Jun Fan
In this paper, a novel detection method based on luminescence resonance energy transfer (LRET) system for sensitive detection of Mn 2+ ions has been proposed. The positively charged upconversion nanoparticles capped with polyethyleneimin (PEI-UCNPs) and negatively charged Ag NPs capped with tripolyphosphate (P 3 O 10 5− -Ag NPs) were bound through electrostatic interaction . They were used as energy donors and acceptors, respectively. The green upconversion luminescence could be quenched because of a good overlap between the UCNPs emission and the Ag NPs absorption spectra . Nevertheless, the LRET was disrupted and the green upconversion luminescence was restored in the presence of Mn 2+ because of the coagulation of P 3 O 10 5− -Ag NPs. Thus, the relative luminescence intensity increased as the concentrations of Mn 2+ increased. The response is linear to the concentrations of Mn 2+ in the range from 0.2 to 5 μM, and the detection limit is evaluated to be 150 nM (S/N = 3). This probe was easy to operate with satisfactory selectivity and excellent sensitivity, which would be able to satisfy the requirements of Mn 2+ -related detection.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Xu Yang,Jiaju Wu,Ying Liu,Miao Yu,Yong Li,Liping Zhao,Cheng Li,Maohui Yuan
Yb 3+ -Mn 2+ dimer based upconversion nanocrystals (UCNCs) have great prospects in biological and photonic applications. In this work, the broadband upconversion luminescence (UCL) of Yb 3+ -Mn 2+ dimer in perovskite nanocrystals is systematically engineered under multi-wavelength excitations. Under the excitation of 980, 940 and 915 nm lasers, KCdF 3 :Yb 3+ /Mn 2+ UCNCs generate yellow broadband UCL from Yb 3+ -Mn 2+ dimer at room temperature and achieve maximum intensity as Mn 2+ concentration reaches 7.5 mol%. By introducing Er 3+ ions into the KCdF 3 host matrix, the UCL color can be further tuned to pure red with high spectral purity, and the red-to-green (R/G) UC intensity ratio is promoted dramatically. The bidirectional energy transfer (ET) processes between Yb 3+ -Mn 2+ dimer, Mn 2+ and Er 3+ ions facilitate color modulation, supported by power dependence and lifetime measurements. Especially, the ET efficiency is evaluated under the multi-wavelength excitations, confirming the high efficiency of ET processes from Yb 3+ -Mn 2+ dimer to Er 3+ ions. Moreover, the obtained KCdF 3 :Yb 3+ /Mn 2+ /Er 3+ UCNCs present a maximum magnetization intensity of 2.01 emu/g when Mn 2+ concentration reaches 98.5 mol%. Both the tunable UCL and excellent paramagnetism properties indicate that these KCdF 3 :Yb 3+ /Mn 2+ /Er 3+ UCNCs have the capability of bifunctional biomarkers of nanomaterials and can be a candidate for bio-related applications.
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Biomaterials Research
·
2024
·
IF 8.1
Mingxiao Fang,Jun Zheng,Jingxue Wang,Chenpeng Zheng,Xiaojing Leng,E. Wen,Pan Li,Haitao Ran,Liang Zhang,Zhigang Wang
The field of immunotherapy, particularly immune checkpoint blockade (ICB), holds immense potential in mitigating the progression of cancer. However, the challenges of insufficient tumor antigen production and the immunosuppressive state in the tumor microenvironment substantially impede patients from deriving benefits. In this research, we present a tumor-microenvironment-modulation manganese-based nanosystem, PEG-MnMOF@PTX, aiming to improve the responsiveness of ICB. Under acidic conditions, the released Mn2+ accomplishes multiple objectives. It generates toxic hydroxyl radicals (•OH), together with the released paclitaxel (PTX), inducing immunogenic cell death of tumor cells and normalizing tumor blood vessels. Concurrently, it facilitates the in situ generation of oxygen (O2) from hydrogen peroxide (H2O2), ameliorating the microenvironmental immunosuppression and increasing the efficacy of immunotherapy. In addition, this study demonstrates that PEG-MnMOF@PTX can promote the maturation of dendritic cells and augment the infiltration of cytotoxic T lymphocytes through activation of the cyclic guanosine 5′-monophosphate–adenosine 5′-monophosphate synthase (cGAS) and interferon gene stimulator (STING) pathways, namely cGAS–STING pathways, thereby heightening the sensitivity to ICB immunotherapy. The findings of this study present a novel paradigm for the progress in cancer immunotherapy.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Guangliang Lu,Rao Qin,Dabiao Zhai,Tianqi Wan,Jiangang Jiang,Dan Zhang,Ping Zhang,Yiping Wang,He Wang
The development and comparison of Latent Fingerprint Patterns (LFPs) constitute critical components of research in fingerprint detection and identification. However, the development of nanomaterials visualization and digital algorithms for LFPs analysis are mostly studied independently, resulting in inaccurate LFPs. This research synthesized a series of efficient red-emitting NaYF 4 :20 %Yb, 2 %Er, x %Mn ( x = 0, 5, 10, 15, 20, 25, 30, 35, and 40) upconversion nanoparticles (UCNPs) for image development, which were combined with a digital algorithm for accurate LFP recognition. The eightfold increase in luminescence intensity of NaYF 4 :Yb, Er, 30 %Mn at 653 nm effectively avoids interference from biological tissue fluorescence. This improvement is credited to the efficient reverse energy transfer mechanism between Er 3+ and Mn 2+ ions, specifically the transition sequence 4 S 3/2 (Er 3+ ) → 4 T 1 (Mn 2+ ) → 4 F 9/2 (Er 3+ ). Furthermore, a MATLAB program was employed to process the fluorescent images of LFPs developed using the UCNPs nanophosphors, achieving a high matching score of 90.09 % for the optimized sample, significantly outperforming traditional benchmarks. These results demonstrate the superior effectiveness of the NaYF 4 :Yb, Er, 30 %Mn nanophosphor, combined with digital processing algorithms, for practical LFP recognition applications.
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Advanced Optical Materials
·
2025
·Vol. 13
·期 6
·2402515
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IF 7.2
Ruichen Xu,Biao Zheng,Xiaochen Fang,Xiaolong Sun,Jinquan Hong,Hai Huang,Weiguo Wang,Jun Wang
Multifunctional optical materials with temperature sensing and anti-counterfeiting properties play an essential role in the commercial applications. Herein, Mn 2+ /Nd 3+ co-doped Cs 2 AgInCl 6 (CAIC) lead-free double perovskites (DPs) is synthesized through a hydrothermal method, which exhibits visible to near-infrared (NIR) luminescence and reversible photochromic properties from yellowish to dark purple. The mechanism investigations on the photoluminescence and photochromic phenomena reveal that the incorporation of Mn 2+ ions not only acts as an intermediary in the energy transfer process from the host exciton to Nd 3+ ions, but also plays a pivotal role in the reversible photochromic response. The temperature-dependent luminescence, attributed to the contrasting thermal responses of Mn 2+ and Nd 3+ ions, enables precise temperature sensing via the fluorescence intensity ratio method. In addition, the integration of visible red emission, NIR luminescence, and photochromic properties in a single CAIC: Mn 2+ /Nd 3+ DPs, offers a multilevel anti-counterfeiting strategy. The multifunctional CAIC: Mn 2+ /Nd 3+ DPs would open up new avenues for advanced optical applications, particularly in the realms of temperature sensing and security anti-counterfeiting.
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CHEMISTRY-A EUROPEAN JOURNAL
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2025
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IF 3.7
Yueyue Wu,Lan Liu,Zifan Li,Jiayi Xie,Zixin Wang,Guo Fang,Keyan Li,Zhenhui Tao,Xin Li,Fei Xiu,Juqing Liu
Graphical With the synergy of Mn 2+ and ODA codecoration, CDs with ultrabroadband and efficient yellow fluorescence in the solid state were synthesized through a simple one-step solvothermal process. These synthetic phosphors exhibit a production yield of 80%, an FWHM of 98 nm, and a solid-state quantum yield up to 62.8%, allowing for high-CRI white LEDs in green and health lighting. Exploiting environment-friendly and efficient phosphors is crucial to constructing high-quality and sustainable white light-emitting devices. Here, we demonstrate a facile and high-yield approach to synthesize Mn 2+ /octadecylamine (ODA)-codecorated carbon dots (CDs) with ultrabroadband and efficient yellow fluorescence in the solid state. The dots are prepared from anhydrous citric acid (CA), 1-ODA, and manganese acetate through a simple one-step hydrothermal process, with a production yield of 80%, a full width at half maxima (FWHM) of 98 nm, and a solid-state quantum yield up to 62.8%. Utilizing the synthetic CDs powder as a phosphor to directly coat on a blue light-emitting chip, the device exhibits warm white emission, with a high color rendering index (CRI) of 88, correlated color temperature (CCT) of 4215 K, and Commission International de l'Éclairage (CIE) coordinates of (0.33, 0.31), endowing great potential applications in green and health lighting.
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Nanomaterials
·
2025
·Vol. 15
·期 14
·1117
·
IF 4.3
Xiaomeng Wang,Siyi Wei,Jiaping Zhang,Jiaren Du,Yukun Li,Ke Chen,Hengwei Lin
Mn2+-doped phosphors emitting green light have garnered significant interest due to their potential applications in display technologies and solid-state lighting. To facilitate the rapid synthesis of high-performance Mn2+-activated green phosphors, this research optimizes a microwave-assisted solid-state (MASS) method for the preparation of Na2ZnGeO4:Mn2+. Leveraging the unique attributes of the MASS technique, a systematic investigation into the applicability of various Mn-source precursors was conducted. Additionally, the integration of the MASS approach with traditional solid-state reaction (SSR) methods was assessed. The findings indicate that the MASS technique effectively incorporates Mn ions from diverse precursors (including higher oxidation states of manganese) into the crystal lattice, resulting in efficient green emission from Mn2+. Notably, the photoluminescence quantum yield (PLQY) of the sample utilizing MnCO3as the manganese precursor was recorded at 2.67%, whereas the sample synthesized from MnO2exhibited a remarkable PLQY of 17.69%. Moreover, the post-treatment of SSR-derived samples through the MASS process significantly enhanced the PLQY from 0.67% to 8.66%. These results underscore the promise of the MASS method as a novel and efficient synthesis strategy for the rapid and scalable production of Mn2+-doped green luminescent materials.
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CRYSTAL GROWTH & DESIGN
·
2025
·
IF 3.4
Biao Xu,Wanyuan Li,Chengyu Ni,Wubin Dai
Unlike static anticounterfeiting that is easily replicated, dynamic multimode photoluminescence (PL) technology has a brighter application prospect in anticounterfeiting/encryption. Yet, the majority of dynamic PL phosphors currently still rely solely on the optical storage mechanism, resulting in a scarcity of diversification, and can easily be decoded. Herein, a series of SrGa2Si2O8: Mn2+/Cr3+ (SGS: Mn/Cr), synthesized via a facile solid-state reaction, is designed to explore interrelationships among entangled changes in the host structure, crystallographic site occupancy, dynamic multimode PL, and multiapplications in anticounterfeiting, encryption, and optical thermometry, based on theoretical calculations and experimental analyses. Although pristine SGS only provides 7(Sr)- and 4(Ga, Si)-fold sites for dopants to occupy, highly efficient characteristic broadband red-NIR emission at ∼765 nm from Cr3+ in 6-fold crystallographic position is obtained as a result of fine-tuning of the local site from [GaO4] to [Ga(Cr)O6] and the close ionic radius in the same valence. Based on the spectral superposition of Mn2+ simultaneously from [Ga(Mn)O4], [Sr(Mn)O7], and Mn–Mn dimers, broadband PL in the green region with a summit of ∼530 nm is gained. The green- and red-NIR afterglows from Mn2+ and Cr3+ with wide and continuous multiple traps are also studied. Owing to the combined PL from the codoped SGS: Mn/Cr, which shows strong correlations with excitation wavelength, doping content, composition, temperature, and detecting time, dynamic multimode PL is realized under distinct test conditions, and the corresponding applications are achieved in the laboratory. This study gives new cogitations in structural adaptabilities for Cr-activated phosphors and their related actual applications.
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DESALINATION
·
2025
·
IF 9.8
Yan Feng,Weitong Liu,Chengzhi Wang,Su Sun,Shuo Zhang,Yuxi Liu,Juan Tan
The sustainable management of phosphorus, a vital yet scarce resource, is severely challenged by its excessive discharge into water bodies, which causes eutrophication. Achieving ultralow phosphate concentrations while enabling efficient recovery demands advanced materials that transcend the capacity and functionality limits of conventional adsorbents. Herein, we report a rationally designed MnLa-layered double hydroxide (LDH) with synergistic redox-acid bifunctional sites for self-regenerative phosphate capture and recovery. This material achieves an exceptional adsorption capacity of 108.87 mg P/g and reduces phosphate to trace levels below 0.012 mg/L, surpassing stringent eutrophication thresholds. Crucially, the MnLa-LDH exhibits self-enhanced functionality: the La 3+ acid sites provide strong Lewis acidity for specific inner-sphere complexation, while the adjacent Mn 2+ /Mn 3+ redox couples act as a molecular engine to dynamically regenerate surface hydroxyl groups, sustaining high activity over multiple cycles. Systematic characterization confirms that phosphate uptake triggers a dynamic structural self-optimization, remarkably increasing the specific surface area by 112.6 %. The material demonstrates broad pH adaptability, high selectivity, and outstanding reusability (87.5 % capacity retention after 10 cycles) with 92.3 % phosphate recovery. This work provides a novel design paradigm for smart environmental functional materials based on synergistic site engineering, paving the way for sustainable water treatment and closed-loop resource circulation.
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CERAMICS INTERNATIONAL
·
2024
·Vol. 51
·期 7
·9292-9300
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IF 5.1
Yue Zhong,Tao Su,Jing Xie,Chao Wang,Wenming Wang,Yan Pan,Xiantao Wei,Yong Li
Mn-doped phosphors exhibiting self-reduction behavior have garnered significant attention in the study of luminescent materials due to the defects generated during the self-reduction process and their unique luminescent behavior. In this paper, LiScGeO 4 red phosphors activated by the self-reduction of Mn 4+ to Mn 2+ were synthesized by high-temperature solid-state reaction in an air atmosphere. The defects generated during the self-reduction process were leveraged to attain exceptional anti-thermal quenching characteristics, with luminescent intensity at a high temperature of 430 K being 1.23 times compared to that at room temperature of 300 K. In addition, a peculiar phenomenon occurred where the emission peak initially blueshifts and subsequently redshifts with the increasing temperature. This study includes an analysis of the Rietveld-refined lattice parameters and surface micromorphology of the samples. The theoretical energy gap of the perfect LiScGeO 4 matrix was calculated using density functional theory . Furthermore, the unique emission peak shift characteristics of Mn 2+ were elucidated through the interaction between Mn 2+ ions and the strength of the crystal field . Utilizing a defect model, the self-reduction mechanism and the anti-thermal quenching behavior were clarified. These findings will enhance the understanding of the effects of crystal defects and ion pair interactions on luminescent materials , and encourage further explorations of self-reducing phosphors to develop new high thermal stability phosphors for practical applications.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2026
·
IF 5.9
Qiwei Zhong,Yueyang Liu,Jiayu Song,Yuchao Cui,Haozhe Li,Li Zhao
Fe/Ti co-doping converts the P2 phase to the OP4 phase and suppresses the undesirable P2-O2 phase transition. • Fe/Ti co-doping breaks the Na + /vacancy ordering and improves sodium ion transport capability. • Ti doping can shorten the TM-O bonds and lengthen the Na-O bonds. P2-type Na 2/3 Ni 1/3 Mn 2/3 O 2 is regarded as a promising cathode material for sodium-ion batteries owing to its high specific capacity and low cost. Nevertheless, its practical application is hindered by irreversible structural degradation and rapid capacity decay associated with the detrimental P2–O2 phase transition during deep Na + extraction. In this work, Fe and Ti are co-incorporated into Na 2/3 Ni 1/3 Mn 2/3 O 2 via a sol-gel method to enhance structural stability. Rietveld refinement of X-ray diffraction (XRD) patterns indicates that Ti doping shortens TM–O bonds and enlarges Na + diffusion channels by increasing Na-O distances, thereby enhancing structural stability and Na + transport kinetics. In situ XRD analyses reveal that Fe/Ti co-doping regulates the phase transition pathway from the irreversible P2–O2 phase transition to a reversible P2–OP4 phase transition, effectively mitigating structural degradation during cycling. Electrochemical measurements demonstrate that optimized Fe/Ti co-doping enhances the overall electrochemical performance. The optimized composition, Na 2/3 Ni 1/4 Fe 1/12 Mn 7/12 Ti 1/12 O 2 , exhibits excellent cycling stability with a capacity retention of 82.33% after 50 cycles at 0.2 C, and delivers a specific capacity of 61.43 mA h g −1 at a high rate of 5 C. This study demonstrates that the combination of sol-gel synthesis and co-doping engineering provides an effective strategy for designing high-performance cathode materials for sodium-ion batteries.
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