Catalysts
·
2025
·Vol. 15
·期 10
·933
·
IF 4
Junxi Tang,Yue Zhang,Jun Yin,Yiwen Chen,Guocheng Deng,Yulong Jin,Jie Xu,Bing Xue,Fei Wang
The utilization of carbon dioxide (CO2) for synthesizing value-added chemicals represents a promising environmentally sustainable strategy. Herein, we synthesized a series of Mn2O3catalysts derived from metal-organic frameworks (MOFs) incorporating three different ligands—homophthalic tricarboxylic acid (H3BTC), 1,4-benzenedicarboxylic acid (H2BDC), and a combination of polyvinyl pyrrolidone (PVP) with H3BTC—via a hydrothermal method for ethylene urea (EU) production from CO2and ethylenediamine (EDA). The Mn2O3catalyst derived from the H3BTC+PVP ligand system (designated MnTP) demonstrated superior catalytic performance, achieving 97% EDA conversion and 97% EU selectivity under mild conditions (100 °C, 1 min), which surpassed all previously reported catalysts under comparable conditions. The enhanced activity originated from structural improvements induced by the H3BTC+PVP precursors, particularly the promotion of oxygen vacancies and Mn3+species, thereby facilitating efficient CO2activation and binding. This work establishes a novel strategy for the sustainable conversion of CO2into high-value cyclic ureas through rational catalyst design.
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Huixian Xie,Liping Tan,Zhuo Yao,Jiaxiang Cui,Xiaokai Ding,Zuhao Zhang,Dong Luo,Zhan Lin
Li-rich Mn-based layered oxides are proposed to be candidates for high-energy Li-ion batteries. However, their large-scale production is still hampered by poor rate capability and severe voltage decay. It was mainly attributed to the irreversible oxygen loss, which induces transition metal ion migration, electrolyte consumption, and structural evolution. Herein, we propose an effective strategy of phosphorylation, in which the phosphate ion is induced to remove the surface labile oxygen. It urges the Li2MnO3 component to transform to the spinel-like structure and promotes the anionic redox process, thus facilitating lithium-ion diffusion and improving structural stability. As a result, the Li2MnO3 component is more prone to be activated, with the capacity increased by 18% in comparison with the pristine one. It also exhibits a superior capacity retention of 86.1% after 150 extended cycles and better rate performance delivering a capacity of 148.1 mA h g–1 even at 10 C. The effective phosphorylation opens a new way to tune anion redox chemistry and obtain structurally stable materials.
研究领域:
材料科学
·
电化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yihao Liu,Nian Ran,Riyue Ge,Jianjun Liu,Wenxian Li,Yingying Chen,Lingyan Feng,Renchao Che
Transition metal phosphides (TMP) show great potential to alternative noble metal based electrocatalysts for oxygen evolution reaction (OER) electrolysis but the still unsatisfactory catalytic activity hinders its practical application. Therefore, it is of much significance to rationally design TMP electrocatalysts for achieving high-efficiency OER. Here, we design Mn-doped cobalt phosphide (Mn-CoP) porous nanosheets for highly active OER through the in-situ metal acetate hydroxide transformation and subsequent phosphidation treatment. Benefiting from synergistic effects of the porous structure, high density of active sites and improved charge-transfer capability, the optimized Mn-CoP serving as a pre-catalyst shows an impressive alkaline OER performance with a low overpotential of 288 mV at the current density of 10 mA cm −2 and high stability. Post-electrolysis characterizations show the conversion from Mn-CoP to vertical Mn-CoOOH hexagonal nanosheets during OER, in which the transformed Mn-CoOOH not only provide extra active sites, but serve as the highly active species. Density functional theory (DFT) calculations reveal that Mn doping can increase the gap states near the Fermi level of active O sites, endowing facilitated deprotonation of OH* to O* and reducing the energy barrier of rate-determining step. This protocol provides a novel insight for the construction of highly efficient TMP water oxidation electrocatalysts.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
LANGMUIR
·
2026
·
IF 4.4
Chao Ge,Yunlan Gu,Bin He,Yanqing Wang,Yawen Tang,Tongfei Li
The advancement of catalysts that are both platinum-group-metal (PGM)-free and iron-free is essential for the oxygen reduction reaction (ORR), which is kinetically slow, particularly in anion-exchange membrane fuel cells (AEMFCs). One of the primary obstacles lies in achieving adequate activity and stability within the membrane electrode assembly (MEA) under real-world hydrogen-air operating conditions. Herein, an effective MnN4 site encased within N-doped carbon nanofibers (denoted as MnN4@N-CNFs) is designed for efficient ORR electrocatalysis. Benefiting from the electronic structure modulation of MnN4 moieties through strong interfacial coupling with the carbon matrix, and structural advantages of the 3D hierarchical porosity synergizing with N-doped carbon-MnN4 coordination systems, the as-resultant MnN4@N-CNFs demonstrate a high half-wave potential of 0.89 V, outstanding durability, and impressive methanol tolerance under alkaline environments, outperforming commercial Pt/C and a diversity of reported counterparts. Notably, the engineered catalyst demonstrates remarkable fuel cell performance with a peak power density of 222.0 mW cm–2 during practical AEMFC operation, while maintaining stable operation for over 15 h, representing a 3-fold enhancement over conventional Pt/C-based counterparts. This study establishes fundamental design principles for high-efficiency AEMFCs through atomic-level engineering of precisely coordinated metal–N–C active sites, providing a robust framework for next-generation electrocatalyst development.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Jiajia Chen,Baobao Bai,Juan Lei,Peng Wang,Shuang Wang,Jinping Li
Mn 3 O 4 catalysts have shown great potentials for toluene catalytic oxidation for the spinel structure and weak metal oxygen bonds. In this work, Mn 3 O 4 and Mn 2 O 3 catalysts were obtained by using Mn-MOFs with different ligands as precursors. It was found that the reduction of hydroxyl groups in 2,5-dihydroxyterephthalic acid was favorable for the preparation of Mn 3 O 4 under the proper temperature range. The Mn 3 O 4 -MOF-74–300 catalyst exposed the highest Mn 3+ , O ads /O latt and reducing capacity. Herein, the Mn 3 O 4 -MOFs-74–300 catalyst exhibited excellent performance for toluene oxidation, which could achieve 90% toluene conversion at 218 ℃ (toluene concentration = 1000 ppm and SV = 20000 mL·g −1 ·h −1 ). Moreover, the Mn 3 O 4 -MOFs-74–300 catalyst exhibited high stability, circulation performance and water resistance in the catalytic test.
研究领域:
材料科学
·
环境科学
·
催化化学
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DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Jingyu Ren,Yanzhong Zhen,Jian Wang,Jie Li
In this study, caffeic acid (CA) was degraded by electrical discharge plasma combined with Mn doped CoOOH catalyst. Doping of Mn significantly improve the catalytic activity of CoOOH. CA degradation efficiency was 75.6% with dielectric barrier discharge treatment for 10 min, and it reached 97% using CoOOH as the catalyst at the same treatment time. CA was 100% degraded with only 8 min using Mn/CoOOH as the catalyst. The introduction of Mn into the lattice of CoOOH induced the formation of oxygen vacancy , causing part of coordinate number of Co decreased from 6 to 5, and thus produces unsaturated Co to be the Lewis acid sites. Lewis acid sites (unsaturated Co) could coordinate with O 3 and H 2 O 2 and break their chemical bonds to form O and –OH. Assisting in the conversion of O 3 to ·OH was the main role of H 2 O 2 in the catalytic process. The degradation products and pathway of CA were studied by three-dimensional fluorescence, liquid chromatograph-mass spectrometer and density functional theory calculations.
研究领域:
环境科学
·
催化化学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Shengfeng Yang,Qingchao Xiao,Bin Li,Tao Zhou,Qihong Cen,Zewei Liu,Yue Zhou
Heavy metal contamination, particularly by lead and cadmium, poses a significant environmental challenge. Indiscriminate disposal of crop residues exacerbates environmental concerns. In this study, broad bean straw was utilized to produce biochar (BC), and further modifications were made using FeCl 3 -6 H 2 O and KMnO 4 to obtain Iron-Manganese Modified Biochar (FMBC) for remediating cadmium and lead-contaminated soil. Results show that both BC and FMBC increased soil pH, available phosphorus, and potassium compared to the control groups. Adding 5 % BC led to a notable reduction of 60.98 % in available cadmium and 51.63 % in available lead. Simultaneously, FMBC decreased active cadmium and lead by 57.51–73.73 % and 52.25–69.87 %, respectively. Furthermore, FMBC decreased the content of cadmium and lead in the unstable state while increasing content in the residual state, demonstrating its ability to reduce accumulation in plant tissues. FMBC adsorption mechanisms primarily involve surface complexation and co-precipitation, where oxygen-containing functional groups form stable complexes with free cadmium and lead ions. In conclusion, FMBC proved to be an effective, environmentally friendly soil remediation agent with strong adsorption capabilities and a prolonged shelf-life. This provides a promising solution to alleviate the pollution of heavy metals such as cadmium and lead in soil.
研究领域:
环境科学
·
土壤学
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DOI
高影响因子
CHEMICAL ENGINEERING & TECHNOLOGY
·
2015
·Vol. 38
·期 2
·291-296
·
IF 2.442
Chen Zhou,Yexin Zhang,Lingjun Hu,Hongfeng Yin,Wei Guo Wang
Mn-doped La 0.8 Sr 0.2 CoO 3 perovskite oxides (La 0.8 Sr 0.2 Co 1– x Mn x O 3 ; x = 0, 0.1, 0.3, 0.5) were synthesized by a modified sol-gel method. The phase-pure oxides were obtained. CoO and carbonates were formed on the surface of La 0.8 Sr 0.2 CoO 3 . With increasing doping content, these impurities were reduced while the stability of the perovskite structure was improved. The valence state of B-site ions and the amount of absorbed oxygen were influenced by Mn doping. The catalytic activity of the perovskite catalysts was investigated for CO oxidation and simultaneous removal of CO, C 3 H 8 , and NO. For CO and NO removal, La 0.8 Sr 0.2 Co 0.9 Mn 0.1 O 3 exhibited the best performance. For C 3 H 8 removal, the reactivity was promoted linearly with the doping content. The structure-activity relationship is also discussed.
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Boying Wang,Hao Wang,Jiantao Wang,Chaolong Li,Feng Wang,Chunli Diao,Haiwu Zheng
Dielectric thin film capacitors are expected to be a promising candidate for high-performance energy storage devices due to their high power density, fast charge/discharge speed, and excellent stability. Nevertheless, it remains a challenging endeavor to develop dielectrics with excellent energy storage density comparable to that of commercial batteries. In this work, lead-free 0.8SrTiO 3 -0.2BiFeO 3 (0.8STO-0.2BFO) thin films with coexisting amorphous and nanocrystalline structure were prepared by a sol-gel method. The heat-treatment temperature was adjusted to form polar-nano regions, thereby modulate the breakdown strength and dielectric polarization, and increase the energy storage density. The electric potential, electric field, and current density of the films with different amorphous/crystalline volume fractions were evaluated by the finite element simulation to further verify that the proper crystallization can result in the improved polarization performance and increased breakdown strength of the films, which are beneficial to the enhancement of energy storage performance. Through structural tailoring, the 0.8STO-0.2BFO film annealed at 550 °C demonstrates the optimal energy storage properties with a giant discharge energy storage density of 65 J/cm 3 and high efficiency of 75% at room temperature. Simultaneously, a broad temperature stability (20–160 °C), superb operating frequency stability (20 Hz-2 kHz), and excellent fatigue endurance (6.3 ×10 5 ) are observed without appreciable degradation of the energy storage performance. The excellent energy storage performance indicates a widespread potential of 0.8STO-0.2BFO films in pulse power applications, such as consumer electronics, microelectronics, and medical devices .
研究领域:
材料科学
·
能源存储技术
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DOI
高影响因子
Journal of Energy Storage
·
2026
·
IF 10.7
Yang Wang,Jing Wang,Jiahuan Luo,Chuanhao Luo,Xu Deng,Ying Liu,Huihui Zhao,Jiayi Ren,Yubiao Xu,Shaojie Zhu,Wanting Shi,Zhenjun Liu,Hao Liu,Rui Hao,Ning Fu
Aqueous zinc‑iodine batteries (AZIBs) are considered promising candidates for large-scale energy storage owing to their high theoretical energy density and intrinsic safety. However, the practical performance is severely limited by sluggish I 2 redox kinetics and the shuttle effect of soluble polyiodide. In this work, a curvature engineering strategy is developed for Mn-N 4 single-atom sites, in which the introduction of C I bonds induces a surface-contracted structure, leading to the formation of a Mn-NC-I configuration. This structural modulation breaks the geometric symmetry of the Mn-N 4 sites and redistributes the local electronic density, enabling directional halogen-bond interactions with polyiodide. As a result, I 2 are effectively anchored, polyiodide shuttling is suppressed, and the I 3 − /I − conversion kinetics are significantly accelerated. Benefiting from enhanced I 2 confinement, and catalytically active Mn centers, the Mn-NC-I/I 2 cathode delivers a high reversible capacity of 148.4 mAh g −1 at 0.1 A g −1 , excellent rate capability, and an ultralow capacity decay rate of 0.0016% per cycle over 20,000 cycles at 10 A g −1 . This study elucidates the critical role of curvature engineering in regulating Mn-N 4 mediated I 2 redox chemistry and provides a viable design principle for high-performance single-atom catalysts in AZIBs.
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高影响因子
FUEL
·
2022
·
IF 8.035
Mingqiang Chen,Wei Dai,Yishuang Wang,Zhiyuan Tang,Hong Li,Chang Li,Zhonglian Yang,Jun Wang
Lignin catalytic depolymerization (LCD) into liquid fuels and aromatic chemicals in supercritical ethanol systems is one of the most effective strategies for efficient utilization of biomass resources. In this study, a series of sepiolite (SEP) supported Mo-Mn catalysts with different Mn/Mo ratios were prepared and applied to LCD. Experimental results for lignin and 2-phenoxy-1-phenyl ethanol (PP) confirmed that Mo/Mn species promoted the breakage of β-O-4 bonds, Mn additive effectively inhibited the alkylation of intermediates, and Mn/Mo ratios distinctly affected the yields of lignin oil (LO) and guaiacols. All as-prepared Mn-Mo/SEP catalysts achieved approximately 100 % conversions of lignin and PP. Various characterization results demonstrated that Mn/Mo ratios could regulate the particle sizes of metal oxides as well as the concentration of oxygen vacancies (O V ) and surface acidic sites. In 3Mn1Mo/SEP, the appropriate interaction among SEP , Mn and Mo species reduced the particle sizes of metal oxides and rendered the crystalline phase structure in a relatively complex state, which undoubtedly generated massive steps/corners on its surface and then enhanced the hydrogenation reaction. Furthermore, the 3Mn1Mo/SEP contained many O V and suitable distribution of Lewis and Brønsted acid sites, which facilitated the adsorption of oxygen-containing intermediates and further hydrogenation and deoxygenation. Therefore, 3Mn1Mo/SEP achieved 45.7 % of LO yield with an HHV of 32.31 MJ/Kg and the highest selectivity to phenols (85.61 %) and yield of guaiacols (308.9 mg/g lignin). In addition, the plausible reaction network for LCD was proposed based on the results of experiments and characterizations.
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高影响因子
CATALYSIS COMMUNICATIONS
·
2022
·
IF 3.51
Haoxuan Wei,Jujiao Zhao,Md. Hasibur Rahaman,Quanfeng Wang,Jun Zhai
In this study, the catalytic activity of soluble Mn(III) ions, soluble Mn(III)-pyrophosphate (PP), and solid Mn(III) (α-MnO 2 ) towards peroxymonosulfate (PMS) activation was investigated through carbamazepine (CBZ) degradation. The degradation efficiency of CBZ was negligible when soluble Mn(III) ions or Mn(III)-PP were used as catalysts, while 99.7% of CBZ was degraded in the α-MnO 2 /PMS system with no soluble Mn(III) ions detected. The degradation efficiency of CBZ reduced by 18% with the solid Mn(III) content decreasing. Hence, the solid Mn(III) made the major contribution to PMS activation. This study supported a better understanding of the role of Mn(III) in PMS activation.
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高影响因子
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