Catalysis Science & Technology
·
2022
·Vol. 12
·期 13
·4157-4168
·
IF 6.177
Rui Huang,Li Luo,Wei Hu,Zhixin Tang,Xing Ji,Leqi Chen,Zhaoshi Yu,Yunhuai Zhang,Dan Zhang,Peng Xiao
Mn-Based metal oxides have shown promising performance in catalytic oxidation of toluene due to the mixed Mn3+ and Mn4+ valences on the surface. Herein, a series of Co–Mn catalysts were synthesized by adjusting the redox precipitation pH to explore the effect of pH on Mn3+, Mn4+ and the surface adsorbed oxygen species when applied for toluene combustion. The Co–Mn-12 catalyst fabricated at pH = 12 displayed excellent catalytic activity and stability for the toluene oxidation of which the T90 at 20 000 mL g−1 h−1 was 208 °C. The toluene conversion could be maintained at around 100% even with the introduction of 10 vol% H2O at 230 °C. We found the appropriate pH for the promotion of the generation of more Mn3+ and Co3+ ions, which were conducive to the formation of oxygen vacancy clusters and resulted in more adsorbed oxygen species generated on the catalyst surface. Moreover, in situ DRIFTS spectra displayed that the existing high valence metal ions and oxygen vacancy clusters facilitated the CC breaking of aromatic rings and the formation of maleic anhydride in the oxidation process. Therefore, Co–Mn-12 demonstrated the best catalytic activity and water-resistance, illustrating that it is an efficient potential industrial catalyst for removing toluene.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Fan Tang,Yu-Wei Zhao,Yu Ge,Yong-Gang Sun,Yu Zhang,Xiu-Lin Yang,An-Min Cao,Jian-Hua Qiu,Xi-Jie Lin
The sluggish kinetic of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) severely hampers the commercial application of electrochemical water splitting, promoting the urgent exploration of high-efficient bifunctional electrocatalysts. Heteroatom doping and structure engineering have been identified as the most effective strategies to boost the catalytic activity of electrocatalysts. Herein, Mn doping and hollow structure were integrated in the design of Co-based transition metal phosphide catalyst to prepare Mn-CoP/Co 2 P nanotubes (denoted as Mn-CP NTs) by a facile template-free method. Confirmed by characterization analysis, the introduced Mn species were in high dispersion in the regular CoP/Co 2 P hollow tubular framework. Such a favorable design in composition and structure effectively boosted the catalytic activity of Mn-CP NTs toward electrochemical water splitting. The Mn-CP NTs showed superior HER and OER activity demonstrated by the low overpotentials of 82 mV ( vs HER) and 309 mV ( vs OER) at the current density of 10 mA cm −2 , as well as the satisfactory durability. When used as both cathode and anode in electrolyzer for overall water splitting, only a low cell voltage of 1.67 V was required for the Mn-CP NTs to drive 10 mA cm −2 , accompanied with excellent stability confirmed by over 50 h test.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2018
·
IF 4.427
Bin Deng,Yating Li,Weihua Tan,Zhaoxi Wang,Ziwei Yu,Shuya Xing,Heng Lin,Hui Zhang
Mn-Zn ferrite (Mn 0.6 Zn 0.4 Fe 2 O 4 ) was prepared by a gel method using spent alkaline Zn-Mn batteries as raw materials and employed as catalyst to degrade bisphenol A (BPA) by electro-enhanced heterogeneous activation of peroxydisulfate (PDS). The effects of initial pH, current density, PDS concentration, and Mn-Zn ferrite dosage on BPA removal were investigated. The formation of reactive radicals was verified by electron paramagnetic resonance (EPR) spectroscopy. The results of radical quenching experiments indicate that surface-bound sulfate and hydroxyl radicals played an important role in BPA removal. The stability of Mn 0.6 Zn 0.4 Fe 2 O 4 catalyst was investigated by cycling experiments, which indicates Mn 0.6 Zn 0.4 Fe 2 O 4 is stable and can be reused. This work also provides an alternative way for the reutilization of spent alkaline Zn-Mn batteries.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xi Chen,Xiaoyan Wang,Ziliang Jia,Chao Yang,Zhihong Liu,Yuexing Wei,Mengxue Wang,Meisheng Liang
K-doped Mn–Ce solid solution catalysts were synthesized using a combination of coprecipitation and hydrothermal methods, demonstrating excellent performance in benzene oxidation. The catalyst K 1 Ce 5 Mn 5 exhibited comparable activity to noble metal catalysts, achieving a 90 % benzene conversion at approximately 194 ℃. Durable tests under dry and moist conditions revealed that the catalyst could maintain its activity for 50 h at 218 ℃ and 236 ℃, respectively. Characterization results indicated that the catalyst’s enhanced activity resulted from the weakened Mn–O bonding caused by the introduction of K + , facilitating the activation of oxygen and its involvement in the reaction. CeO x , the main crystalline phase of Mn–Ce solid solutions, provided abundant oxygen vacancies for capturing and activating oxygen molecules for the weakened Mn–O structures. This conclusion was further supported by partial density of state analysis from density functional theory computations, revealing that the introduction of K + weakened the orbital hybridization of Mn3d and O2p. Finally, in situ diffuse reflectance infrared Fourier-transform spectroscopy ( in situ DRIFTS) studies on Ce 5 Mn 5 and K 1 Ce 5 Mn 5 catalysts suggested that the introduction of K + promoted the conversion of adsorbed benzene. Furthermore, intermediate products were transformed more rapidly for K 1 Ce 5 Mn 5 compared to Ce 5 Mn 5 .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2018
·
IF 3.525
Wenjin Xu,Guangxu Zhang,Hanwei Chen,Guomeng Zhang,Yang Han,Yichuan Chang,Peng Gong
Two series of Mn/beta and Mn/ZSM-5 catalysts were prepared to study the influence of how different Mn precursors, introduced to the respective parent zeolites by wet impregnation, affected the selective catalytic reduction (SCR) of NO by NH 3 across a low reaction temperature window of 50–350 °C. In this study, the catalysts were characterized using N 2 adsorption/desorption, X-ray diffraction, X-ray fluorescence, H 2 temperature-programmed reduction, NH 3 temperature-programmed desorption and X-ray photoelectron spectroscopy. As the manganese chloride precursor only partially decomposed this primarily resulted in the formation of MnCl 2 in addition to the presence of low levels of crystalline Mn 3 O 4 , which resulted in poor catalytic performance. However, the manganese nitrate precursor formed crystalline MnO 2 as the major phase in addition to a minor presence of unconverted Mn-nitrate. Furthermore, manganese acetate resulted principally in a mixture of amorphous Mn 2 O 3 and MnO 2 , and crystalline Mn 3 O 4 . From all the catalysts screened, the test performance data showed Mn/beta-Ac to exhibit the highest NO conversion (97.5%) at 240 °C, which remained >90% across a temperature window of 220–350 °C. The excellent catalytic performance was ascribed to the enrichment of highly dispersed MnO x (Mn 2 O 3 and MnO 2 ) species that act as the active phase in the NH 3 -SCR process. Furthermore, together with a suitable amount of weakly acidic centers, higher concentration of surface manganese and a greater presence of surface labile oxygen groups, SCR performance was collectively enhanced at low temperature.
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Yuxi Liao,Peng Liu,Jun Zhang,Can Wang,Longwen Chen,Dengfeng Yan,Quanming Ren,Xiaoliang Liang,Mingli Fu,Suib Steven L.,Daiqi Ye
Increasing the contact efficiency and improving the intrinsic activity are two effective strategies to obtain efficient catalysts for soot combustion. Herein, the electrospinning method is used to synthesize fiber-like Ce–Mn oxide with a strong synergistic effect. The slow combustion of PVP in precursors and highly soluble manganese acetate in spinning solution facilitates the formation of fibrous Ce–Mn oxides. The fluid simulation clearly indicates that the slender and uniform fibers provide more interwoven macropores to capture soot particles than the cubes and spheres do. Accordingly, electrospun Ce–Mn oxide exhibits better catalytic activity than reference catalysts, including Ce–Mn oxides by co-precipitation and sol-gel methods. The characterizations suggest that Mn 3+ substitution into fluorite-type CeO 2 enhances the reducibility through the acceleration of Mn–Ce electron transfer , improves the lattice oxygen mobility by weakening the Ce–O bonds, and induces oxygen vacancies for the activation of O 2 . The theoretical calculation reveals that the release of lattice oxygen becomes easy because of a low formation energy of oxygen vacancy, while the high reduction potential is beneficial for the activation of O 2 on Ce 3+ -Ov (oxygen vacancies). Due to above Ce–Mn synergy, the CeMnO x -ES shows more active oxygen species and higher oxygen storage capacity than CeO 2 -ES and MnO x -ES. The theoretical calculation and experimental results suggest that the adsorbed O 2 is more active than lattice oxygen and the catalytic oxidation mainly follows the Langmuir-Hinshelwood mechanism. This study indicates that electrospinning is a novel method to obtain efficient Ce–Mn oxide.
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guiyuan Cai,Yu Tian,Lipin Li,Wenxuan Zhang,Rui Huang,Jun Zhang,Qinyu Wang,Hua Xu,Yifeng Zhang
The activation of sulfite [S(IV)] by transition metals, a new generation of advanced oxidation processes, has been widely studied for water purification. However, the application of this process to oxidize and remove arsenite [As(III)] from water through Fe-based S(IV) activation and the associated mechanisms are not fully understood. In particular, rapid removal of As(III) and secondary metal contamination have presented challenges. Herein, we develop a novel sea urchin-like magnetic Fe-Mn bimetallic oxides (FeMnO)-activated S(IV) process to address these issues. Under neutral pH, the FeMnO/S(IV) system achieved a 99.2 % removal of As(III) within only 10 min with residual arsenic concentration below 10 µg/L, and the removed As(III) was fully oxidized to arsenate [As(V)]. Additionally, FeMnO was recyclable and capable of treating actual arsenic-contaminated water. Furthermore, the oxidation mechanism of non-radical active trivalent manganese [Mn(III)] was discovered during the reaction between the FeMnO/S(IV) system and As(III). The FeMnO catalyst activated S(IV) to generate oxysulfur radicals (i.e., SO 5 •– , SO 4 •– and SO 3 •– ), but they were not the primary oxidizing species for As(III). Instead, As(III) oxidation was mainly attributed to the active Mn(III) generated by the electron transfer between the FeMnO catalyst and SO 5 •– radicals. The discovery of active Mn(III) species in this work may provide a new avenue for developing novel Fe-Mn-type adsorbents to purify arsenic-contaminated water.
✓ 已验证
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 11
·1091
·
IF 4
Qiang Zhang,Shiming Qiu,Yanfei Zheng,Yingying Huang
The development of highly active, thermally stable, and low-CO-selective catalysts is critical for practical methanol steam reforming (MSR) to produce high-purity hydrogen for fuel cell applications. In this work, a series of Mn–Cu/Al2Oxcatalysts with varying Mn/Cu/Al molar ratios were synthesized via co-precipitation and systematically investigated to establish the relationship between composition, structure, and catalytic performance. XRD analysis revealed the formation of spinel-type CuAl2O4and MnAl2O4phases, with Mn preferentially occupying octahedral B-sites to form MnAl2O4, thereby inducing lattice distortion and inhibiting grain growth. SEM and TEM–EDS mapping confirmed uniform elemental distribution and a porous nanoscale morphology, while H2-TPR results suggested that increasing the Mn/Cu ratio strengthens Mn–Cu interactions, shifts Cu2+reduction to higher temperatures, and enhances Cu dispersion (up to 26.11 m2/g). XPS analysis indicated that Mn doping enriches Mn3+species and facilitates oxygen vacancy formation, which promotes water–gas shift (WGS) activity and suppresses CO formation. Catalytic testing (240–300 °C) showed that Mn2Cu2Al4Oxachieved the highest methanol conversion while maintaining low CO selectivity; in contrast, reducing the Mn/Cu ratio increased CO selectivity, detrimental to hydrogen purification. Stability tests under continuous steam exposure for 24 h demonstrated minimal activity loss (~2%) and negligible increase in CO selectivity (<1%), confirming excellent hydrothermal stability. The results indicate that tailoring the Mn/Cu ratio optimizes the balance between redox properties and metallic Cu dispersion, offering a promising route to design low-CO, durable catalysts for on-site hydrogen generation via MSR.
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2026
·
IF 19.3
Jian Zhang,Zhiyi Liu,Fang Chen,Jiahui Ye,Longqi Luo,Qing Lang,Liang Chen,Gang Wang
The electrolyte enables reversible Mn plating/stripping from −20 to 120 °C. • A minimum overpotential of 50 mV is achieved for Mn plating/stripping. • Near-integral Coulombic efficiency (99.2–100.3%) is realized in asymmetric cells. • The Mn metal batteries deliver a long cycling life of over 7000 cycles. Mn metal batteries (MnMBs) have attracted widespread attention due to distinct merits of Mn anode on energy-to-price ratio, volumetric capacity and redox potential. However, most MnMBs can only be operated around room temperature, largely constraining their potential application scenarios. In this work, a wide-temperature non-aqueous electrolyte, comprising wide-liquid-range solvents [tetramethylene sulfone (26–285 °C); diglyme (−64–162 °C)] and hybrid solutes (MnCl 2 -AlCl 3 -Mn(TFSI) 2 ), is proposed as the first electrolyte enabling MnMBs to work at −20 to 120 °C. Benefitting from superior stability and high ionic conductivity, the resultant electrolyte allows reversible and dendrite-free Mn plating/stripping with overpotential controlled as low as 50 mV, representing a record in MnMBs. Near integral Coulombic efficiency of Mn plating/stripping is realized in asymmetric Mn cells under different areal capacities. As consequences, the assembled MnMBs show a high average output voltage, a long cycling life of >7000 cycles and wide operation temperature. The wide-temperature electrolyte offers a pathway for designing advanced MnMBs for diverse application scenarios. Download: Download high-res image (183KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Jiacheng Xu,Tiantian Zhang,Yan Sun,Shiyu Fang,Zuliang Wu,Jiali Zhu,Lianxin Dai,Weihua Liu,Buhe Zhang,Junwei Zhang,Shuiliang Yao,Erhao Gao,Jing Li
MnO 2 is a promising catalyst due to its abundant metal valence and good redox ability. Different crystal phases of MnO 2 have different oxygen species, but the relationship between their catalytic activity and crystal structures is unclear. In this study, four MnO 2 catalysts with crystal structures ( α -, β -, γ -, and δ -MnO 2 ) were selected to unveil the roles of terminal-type (Mn O), superoxide-type Mn(-O-) 2 Mn, and bridge-type (Mn-O-Mn) oxygen species in CO oxidation . γ -MnO 2 has the best CO oxidation performance. Density functional theory calculation results show that Mn O on γ- MnO 2 can adsorb CO easier than other two types of oxygen species. Operando TPR-DRIFTS-MS results show that Mn O on the surface of γ- MnO 2 can react with CO to form terminal-type oxygen vacancies (M 2+ =□ 2– ) at low temperatures. Meanwhiles, Mn(-□-)(-O-)Mn and Mn-□-Mn can dissociate O 2 to form Mn O under certain conditions to promote CO oxidation. MnO 2 catalysts with more Mn O oxygen species are of great significance for CO oxidation at a low temperature.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Menglu Xu,Yibing Zhang,Huaqin Yin,Jinnan Wang,Aimin Li,Philippe François-Xavier Corvini
Co-ZFO@Mn-CN with 1 O 2 and O 2 •− as main reactive oxygen species was synthesized for catalytic ozonation , which could efficiently degrade organic pollutants . EPR and XPS analysis indicated that lattice doping of Co induced formation of abundant of OVs, which could provide localized electrons for O 3 activation with the generation of HO 2 • /O 2 •− . 1 O 2 and H 2 O 2 were produced by the recombination of HO 2 • /O 2 •− . DFT calculation demonstrated that H 2 O 2 was deprotonated to generate HOO − , which preferred to form HOO-Mn-N X bonds with Co-ZFO@Mn-CN. Under the attack of O 3 , HOO-Mn-N X bonds were broken with the generation of HO 2 • and HO 3 • /O 3 •− , not only accelerating 1 O 2 production for organics degradation but also avoiding Mn(Ⅱ) sites oxidation . Combining advantages of OVs and HOO-Mn-N X , Co-ZFO@Mn-CN achieved 70–100% mineralization for different organic pollutants . Thus, this work provided a simple and efficient way for enhancing the utilization of O 3 by the synergistic effect of OVs and HOO-Mn-N X bonds, also improving ROS transformation.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2020
·
IF 3.104
Mei Li,Yongcheng Zhang,Haiming Li,Hailing Jiang,Wei Han,Yang Sun
In the present work, cyclic voltammetry (CV), square wave voltammetry (SWV) and chronopotentiometry (CP) were used to investigate the electrochemical coreduction behaviors of La(III) and Mg(II) as well as La(III), Mg(II) and Mn(II) on Mo electrode in LiCl + KCl molten salts. CV and SWV results exhibit that the coreduction mechanism of La (III) and Mg(II) on Mo electrode is that La(III) is reduced and Mg–La intermetallic compound is formed, leading to the deposition potential of La(III) shifting to more positive one. The electrochemical signals pertaining to the formation of metallic La, Mg and Mn as well as Mg–La intermetallic compound are also observed by coreduction of La(III), Mg(II), and Mn(II) in LiCl + KCl molten salt on the inert Mo electrode. However, the electrochemical signals associated with the formation of La–Mn and Mg–Mn alloys are not observed, which means that the depolarization effect of La(III) and Mg(II) does not occur on pre-deposited Mn electrode. The Mg–La–Mn alloys were formed by co-deposition of La(III), Mg(II), and Mn(II) on Mo electrode at various concentration ratios of La(III) and Mg(II). The results of scanning electron microscopy equipped with energy dispersive spectroscopy and X-ray diffraction displays that the Mg–La–Mn alloys are comprised of La–Mg compound Mg 17 La 2 , Mg and Mn phases. The concentration ratio of La(III) and Mn(II) has few effects on the alloy composition .
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）