ACS Catalysis
·
2022
·
IF 13.7
Chunning Zhao,Ao Zhu,Shan Gao,Lijing Wang,Xiang Wan,Ansheng Wang,Wei-Hua Wang,Tao Xue,Shikuan Yang,Deyan Sun,Weichao Wang
A phonon is the medium a bulk material used to exchange energy with the environment and is thus crucial for heterogeneous catalysis. However, a physical correlation between phonons and catalytic processes has not been established yet. Herein, by combining various in situ characterization techniques, we discovered the intrinsic correlations between phonon modes and the vibrations of reactant intermediates during NO oxidation on the mullite catalyst YMn2O5. It was found that the active phonon modes (350 (Ag(5)) and 670 cm–1 (B1g(12))) are strongly correlated with the vibrational frequencies of the adsorbed −O2 and −O–NO2 intermediates. The resulting resonance will transfer the superposed energy (nℏω) of the high-energy phonons to reactants one by one via the unit energy (ℏω) and then increase the vibrational amplitude along the reaction direction, contributing to the increase in the entropy of the surface reactants and thus the reduction of the Gibbs energy of activation. Phonon resonance catalysis (PRCAT) was thus proposed based on this discovery. This work provides insights into the bidirectional selection of catalysts and precise chemical reactions by matching catalyst phonons with reactant vibrational frequencies.
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Qianrui Lv,Chong Li,Lijing Zhang
Developing strategies to modify lead-based metal halide perovskite lattice has become an increasingly important effort because of the need to control fundamental material properties. In this paper, we introduced a flow microreactor for the continuous synthesis of Mn-substituted methylammonium lead tribromide (CH3NH3Pb1–xMnxBr3) quantum dots. The original crystal structure can be retained at high Mn content (x = 0.3). The size and photoluminescence peak of the CH3NH3Pb1–xMnxBr3 quantum dots can be tuned by varying the molar ratio of Pb/Mn. With increasing Mn content, the photoluminescence peak shifted gradually to shorter wavelengths. Mn-substitution also affects the air stability for the quantum dots. CH3NH3Pb0.7Mn0.3Br3 shows the best air stability, and polystyrene can be used to protect the quantum dots. Compared to CH3NH3PbBr3 quantum dots, CH3NH3Pb1–xMnxBr3 quantum dots may prove to be a less toxic and valuable optoelectronic material meeting the requirements for different practical applications.
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ACS Nano
·
2024
·
IF 15.8
Xiaoqian Wei,Shaojia Song,Weiwei Cai,Yunqing Kang,Qie Fang,Ling Ling,Yingji Zhao,Zexing Wu,Xiaokai Song,Xingtao Xu,Sameh M. Osman,Weiyu Song,Toru Asahi,Yusuke Yamauchi,Chengzhou Zhu
The intrinsic roadblocks for designing promising Pt-based oxygen reduction reaction (ORR) catalysts emanate from the strong scaling relationship and activity–stability–cost trade-offs. Here, a carbon-supported Pt nanoparticle and a Mn single atom (PtNP–MnSA/C) as in situ constructed PtNP–MnSA pairs are demonstrated to be an efficient catalyst to circumvent the above seesaws with only ∼4 wt % Pt loadings. Experimental and theoretical investigations suggest that MnSA functions not only as the “assist” for Pt sites to cooperatively facilitate the dissociation of O2 due to the strong electronic polarization, affording the dissociative pathway with reduced H2O2 production, but also as an electronic structure “modulator” to downshift the d-band center of Pt sites, alleviating the overbinding of oxygen-containing intermediates. More importantly, MnSA also serves as a “stabilizer” to endow PtNP–MnSA/C with excellent structural stability and low Fenton-like reactivity, resisting the fast demetalation of metal sites. As a result, PtNPs–MnSA/C shows promising ORR performance with a half-wave potential of 0.93 V vs reversible hydrogen electrode and a high mass activity of 1.77 A/mgPt at 0.9 V in acid media, which is 19 times higher than that of commercial Pt/C and only declines by 5% after 80,000 potential cycles. Specifically, PtNPs–MnSA/C reaches a power density of 1214 mW/cm2 at 2.87 A/cm2 in an H2–O2 fuel cell.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Haoran Wang,Zhaoxia Hou,Hui Zhang,Wensheng Zong,Shuting Yin,Haibo Long,Zhongchao Fu,Nan Wu,Zihui Zhai,Depeng Zhang,Fanshun Meng,Dan Zhou
Aqueous zinc-ion batteries (AZIBs) are considered highly promising next-generation energy storage technologies due to their intrinsic safety, low cost, and high theoretical capacity. Among the potential cathode materials for AZIBs, manganese oxide stands out because of its high theoretical specific capacity, diverse crystal structures, and abundant crustal availability. However, drawbacks of manganese oxide including irreversible phase transitions, low ionic conductivity, and unavoidable Mn 3+ dissolution often result in low capacity and poor cycling stability. Herein, a novel dual-phase material, Mn 2 O 3 /(Co,Mn)(Co,Mn) 2 O 4 (MO/CMO), featuring a meso porous structure and stable phase interface, was facilely synthesized via one-step thermal decomposition of Co 2+ -doped MnCO 3 precursors. The meso pores provide additional active sites, facilitating faster reaction kinetics, while the phase interface effectively suppresses spontaneous Mn 3+ dissolution, resulting in excellent cycling stability. Specifically, the MO/CMO-10 cathode in aqueous electrolyte cell exhibits a high initial specific capacity of 253 mAh g −1 at 0.1 A g −1 , and enhanced cycling stability of 98 mAh g −1 after 2200 cycles at 1.0 A g −1 and an ultra-long cycle life of 63 mAh g −1 over 6800 cycles at 2.0 A g −1 . When assembled in flexible quasi-solid-state ZIBs, the cell maintains a high specific capacity of up to 124 mAh g −1 after 980 cycles at 1.0 A g −1 . Remarkably, the pouch cell sustains stable output even under harsh conditions, indicating promising potential for wearable applications.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yinghao Xue,Wei Teng,Yanyan Chen,Qian Ma,Xiaoqian Chen,Yu Sun,Jianwei Fan,Yuping Qiu,Rongbing Fu
Simultaneous removal of cation (e.g., Pb(Ⅱ), Cd(Ⅱ)) and oxyanion (e.g., As(Ⅴ)) heavy metals have attracted increasing interest for adsorption applications due to the complexity of heavy metal polluted groundwater. Manganese-lanthanum binary oxides immobilized on hydrothermal carbonization carbon (Mn x La 1-x @HTCC) were therefore rationally designed in this work, and the Mn-La oxides immobilized on HTCC exhibited more uniform dispersion compared to bulk phase. In single adsorption systems, superior adsorption of different heavy metals could be achieved by tuning the molar ratio of Mn to La, and Mn leaching was reduced by ∼ 75% compared with Mn@HTCC (without La doping). In the coexisting systems, the simultaneous presence of As(Ⅴ) and Pb(Ⅱ) greatly enhanced adsorption of both two heavy metals, while competition was observed in the coexistence of As(Ⅴ) and Cd(Ⅱ). By analyzing the “release-readsorption” phenomenon of Mn and the variation of Mn valence during adsorption, the different roles of Mn species in the removal of three heavy metals were proposed. Finally, high-speed flow adsorption column experiments confirmed that the Mn x La 1-x @HTCC composite can effectively and continuously adsorb heavy metals accompanied by trace Mn leaching content. Overall, this study indicates the potential of Mn-La carbon composites as a novel adsorbent in groundwater remediation.
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WATER RESEARCH
·
2024
·
IF 11.4
Xuecong Qian,Shilong Wang,Haijun Cheng,Luwei Li,Yun Liu,Jinhao Duan,Da Wang,Jun Ma
Fe(II) and Mn(II) are abundant in groundwater and require operationally simple and efficient method to remove in drinking water treatment. The rapid oxidation of Mn(II) is essential in water treatment. This study investigates the efficiency of Mn(II) oxidation by free chlorine in the presence of Fe(II). The results demonstrate that the presence of Fe(II) significantly accelerates the oxidation rate of Mn(II) by free chlorine under neutral and alkaline conditions. The rapid oxidation of Fe(II) by free chlorine and the presence of Mn(II) promote the formation of in situ Mn(II)-doped ferrihydrite. Kinetic modeling and characterization of Fe(III) oxides confirm that the heterogeneous catalytic effect of the Mn(II)-doped ferrihydrite, rather than manganese oxides or their coupled catalytic effect, is responsible for the enhanced oxidation rates. The doped Mn(II) substitutes the tetrahedral Fe(III) ions in the ferrihydrite, introducing additional negative charges at the doped sites. The increased charge enhances Mn(II) adsorption and lowers its redox potential, thereby accelerating Mn(II) oxidation rate through direct electron transfer with adjacent free chlorine. Additionally, the lepidocrocite formed by the reaction between Fe(II) and dissolved oxygen significantly impedes the catalytic performance. These findings provide new insights into the catalytic co-oxidation mechanism of Fe(II) and Mn(II), and help the optimization of water treatment engineering practices.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Junlei Zhang,Wei Zhao,Shanshan Wu,Renli Yin,Mingshan Zhu
Advanced oxidation processes (AOPs) based on heterogeneous catalytic activated peroxymonosulfate (PMS) have been becoming alternatives to conventional wastewater treatment technologies to directly degrade chemical contaminants. To build dual/multi redox cycles of different metal ions may be an effective means for better PMS activation. Herein, this study designed Mn 3 O 4 /CuBi 2 O 4 with dual redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) to activate PMS for efficiently decomposing and mineralizing diclofenac sodium (DCF). Under optimal reaction conditions, DCF (50 mg/L) was degraded totally within 10 min, and TOC removal rate reached up to 74.3%. The possible mechanism of PMS activation by Mn 3 O 4 /CuBi 2 O 4 was proposed, wherein dual redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) on Mn 3 O 4 /CuBi 2 O 4 effectively facilitated PMS activation to generate · O 2 − , 1 O 2 , SO 4 · − and · OH, which was responsible for DCF degradation. Moreover, combined with degraded products detected by high resolution liquid chromatography coupled to mass spectrometry and corresponding toxic assessment results, the possible degradation pathways of DCF were proposed and the relative toxicity of degraded products was evaluated. This work may be useful for developing stronger heterogeneous activators of PMS to construct more efficient AOPs for purifying wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zhikang Deng,Yongfei Ma,Jinyao Zhu,Chenyu Zeng,Rui Mu,Yifan Liu,Ping Li,Zulin Zhang
Ferrate (Fe (VI)), as a versatile oxidizer, has been widely employed for water treatment. However, the rapid self-decomposition of Fe (VI) diminishes its practical application efficiency. In this study, a novel Mn-modified sludge biochar (MSBC) was synthesized for the first time to activate Fe (VI) and generate highly reactive Fe (IV)/Fe (V) for the rapid removal of sulfamethoxazole (SMX). The results showed that MSBC (0.10 g/L) effectively activated Fe (VI) (100 μM), and 87.39 % of SMX (10 μM) and 40.26 % of total organic carbon (TOC) were removed within 10 min. Notably, raising the solution pH (e.g., from 6.0 to 11.0) would result in decreasing the reactivity of Fe (VI) and a lower removal efficiency of SMX. The quenching, electron paramagnetic resonance and probe experiments suggested that •O 2 – and high-valent iron species (Fe (V)/Fe (IV)) were identified as the major contributions to the removal of SMX. The detailed activation sites of MSBC were –OH and Mn-O, as corroborated by density functional theory (DFT) calculation and characterization. These activation sites facilitated activation of Fe (VI) through efficient electron transfer . The Fukui index indicated that the N, S, and O atom of SMX were the primary attacked sites. Subsequently, five potential degradation pathways were proposed, with the cleavage of the S-N bond being the predominant one. The toxicity of these products was examined using ECOSAR program, revealing that main products showed low toxicity or non-toxicity. The Cl - , SO 4 2- , and NO 3 – had negligible effect on SMX degradation, although excessive concentrations of HCO 3 – and humic acid (HA) showed slightly inhibition. Additionally, the Fe (VI)/MSBC system also effectively removed 87.34 % of sulfadiazine (SDZ) and 93.91 % of sulfamethoxypyridazine (SMP). Overall, this study offered a practical and cost-effective approach for the activation of Fe (VI) and provided new insights to the degradation mechanism.
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ACS Applied Engineering Materials
·
2026
·
IF 3.5
Hao Zhang,Anming She,Junxi Zhang,Zhenxiao Bi,Qing Chen,Hehua Zhu
Cement-based structural batteries offer an attractive pathway for integrating energy storage technologies into civil infrastructure. However, their practical application is severely constrained by capacity degradation caused by the dissolution of trivalent manganese (MnOOH) under alkaline conditions. This study proposes a zeolite-coated cathode strategy to suppress manganese dissolution, thereby achieving highly durable MnO2/Zn cement-based batteries. The zeolite porous framework complex traps free trivalent manganese ions [Mn(OH)6]3– and promotes uniform migration of OH– within the poly(vinyl alcohol)-cement matrix. The optimized MnO2 material enhances electrolyte wetting and reduces interfacial charge transfer resistance. The zeolite-induced effect enables the MnO2 electrode to exhibit highly reversible conversion reactions and stable morphological evolution during cycling. The assembled structural battery achieves high Coulombic efficiency and cycling stability, retaining 56.21% capacity after 300 cycles in the freshly prepared system and 77.09% capacity after 300 cycles following 28 days of cement curing. This study establishes a universal interfacial stabilization strategy through zeolite coating, opening promising avenues for developing energy-storage building materials suitable for long-life infrastructure.
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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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CONSTRUCTION AND BUILDING MATERIALS
·
2025
·
IF 8
Qiang Liu,Guangye Tu,Meng Wu,Guodong Xu,Jianming Gao,Yunsheng Zhang,Cheng Liu
The utilization of metallurgical slag for the partial substitution of clinker to produce blended cement is an effective approach for the harmless and resourceful disposal of industrial solid waste. Nevertheless, the influence of metallurgical slag on the solidification behavior between clinker minerals and heavy metals remains unclear in blended cement. In this study, the blended cement is composed of cement, synthetic amorphous phase (eliminating the influence of physical-chemical characteristics of different metallurgical slags), and different levels soluble Mn. The study applied various characterization methods focusing on the solidification behaviour of Mn in the hydration process of blended cement. The results reveal that Mn exhibits a dual effect on the reaction of C 3 S, with the appearance time of the main peak in the hydration heat curve extending from 10 h to 17 h (when Mn dosage reaches 0.9 wt%). However, with the increase of Mn, the main peak appeared early at 5.6 h. The primary inhibitory factor for the C 3 S hydration reaction is Mn-bearing hydrate phases on the surfaces of cement particles. However, when the soluble Mn content exceeds a certain threshold (2.7 wt% in this study), the clinker reaction is enhanced due to the formation of additional nucleation sites by Mn-hydrate precipitates. Mn is predominantly solidified within the gel-like hydration products and ettringite through lattice confinement and physical encapsulation. The introduction of Mn promotes the formation of ettringite-like products. This reaction consumes gypsum and thus accelerates the secondary hydration of C 3 A. The improved hydration kinetics model is employed to reveal the hydration mechanism of blended cement containing Mn. The hydration process of blended cement follows a diffusion-controlled behaviour, which is influenced by the Mn-precipitation layer. These findings provide comprehensive insights into reaction kinetics and the solidification of heavy metals, contributing to the sustainable application of metallurgical slag in the environment.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2020
·Vol. 31
·期 4
·2887-2894
·
IF 2.22
Liu Yuan,Gu Yi-Jing,Deng Jia-Li,Luo Gui-Yang,Wu Fu-Zhong,Mai Yi,Dai Xin-Yi,Li Jun-Qi
A series of LiFe 1− x Mn x PO 4 /C composites were successfully synthesized through a simple hydrothermal method. The effects of doped Mn on their micro-structures and electrochemical performances were investigated. The XRD results indicate that Mn doping cannot change the olivine lattice type of LiFePO 4 . Appropriate Mn doping can reduce the particle size of LiFePO 4 . The electrochemical performance data show that the electrochemical performances of the composite materials are enhanced at first and then decrease as the doping amount of Mn increases. Both the CV and EIS results illustrate that a small amount of doped Mn will reduce the electrode polarization and electrochemical impedance of the samples and simultaneously improve the electrochemical performance. Among all the samples, the LiFe 0.98 Mn 0.02 PO 4 /C sample has a desirable electrochemical performance, with its specific discharge capacity reaching 156.0 mAh g −1 at a rate of 0.1 C. Even at a high rate of 5 C, it can still reach 110.0 mAh g −1 . All the results indicate that an appropriate amount of doped Mn has an emphatic effect on the electrochemical performance of LiFePO 4 /C.
研究领域:
材料科学
·
电化学
·
能源存储
·
无机化学
·
纳米材料
·
固态化学
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危险品化学品经营许可证（带存储）