Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124763
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IF 7.5
Na Yang,Ruoxuan Bai,Jicheng Han,Fei Gao,Rongkun Jiang,Yiqing Zeng
The selective catalytic oxidation of NH 3 (NH 3 -SCO) is a key technology for controlling NH 3 emissions, but conventional MnO x catalysts suffer from low N 2 selectivity and moderate activity. In this work, a series of MMnO x (M = Mo, W, Sm) bimetallic oxide catalysts were fabricated to regulate the acid–redox properties of MnO x through interactions with secondary metal species for highly efficient NH 3 oxidation. The characterization results show that the introduction of M components can significantly enhance the specific surface area and NH 3 adsorption capacity of MnO x , which generates synergistic adsorption and oxidation functions for NH 3 activation, thereby promoting NH 3 -SCO reaction via internal selective catalytic reduction (i-SCR) pathway. Sm significantly enhances the redox properties and surface oxygen vacancies of MnO x , which facilitates the activation of NH 3 . Consequently, SmMnO x achieves 90% NH 3 conversion at 255 °C (60 °C lower than MnO x ) with > 85% N 2 selectivity. In contrast, W addition suppresses the oxidation ability due to the formation of MnWO 4 species, leading to poor low-temperature activity. Mo addition also forms MnMoO 4 , but the increased surface area, enhanced acidity, and separation of active sites allow MoMnO x to outperform MnO x . These findings indicate that constructing M–Mn binary active sites can regulate the balance between surface acidity and oxidation capability, thereby providing a design strategy for high-performance Mn-based NH 3 -SCO catalysts through the rational selection of secondary metal components to establish complementary adsorption–redox functions.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Qing Wang,Lei Yuan,Jianyu Xu,Ning Zhao,Xingmei Guo,Fangyan Zhu,Ali Tian,Zhenming Zhang,Ge Yin,Junhao Zhang
Crystalline-amorphous CoS 2 -MnO x constructed via deposition-order regulation. • Amorphous MnO x underlayer transports electron and ion flux to electrode surface. • Optimized d-band center on crystalline CoS 2 promoting OER kinetics in seawater. • Electron-enriched surface and dissolved manganate species repelling chloride ions. • Conventional crystalline-on-crystalline anti-chloride overlayer dilemma overcomed. Conventional crystalline-on-crystalline anti-chloride overlayer structures for seawater oxidation electrocatalysis suffer from physical shielding of active sites and limited functional tunability due to lattice constraints. Herein, a crystalline-amorphous CoS 2 -MnO x heterostructure is constructed on graphite felt via a sequential electrodeposition-hydrothermal route, with deposition order mediating precise interface regulation. The as-prepared structure exhibits superior electrocatalytic performance for alkaline seawater oxidation, demanding low overpotentials of 170, 308, and 392 mV to achieve current densities of 10, 100, and 500 mA cm −2 , respectively, together with robust stability. Experimental investigation and theoretical calculation reveal that the heterostructure triggers electron transfer from MnO x to CoS 2 , generating a built-in electric field with interfacial charge redistribution. This modulates the d-band center and accelerates oxygen evolution kinetics. Meanwhile, surface electron enrichment synergizes with released manganate ions to effectively repel chloride ions from approaching and adsorbing. Such directional electron and ion fluxes endow the catalyst with excellent chloride-resisting and oxygen evolution performances in seawater electrolysis. This work demonstrates a facile strategy for constructing crystalline-amorphous heterostructures and elucidates the interfacial engineering mechanism for enhanced seawater oxidation, offering a promising new paradigm for advanced electrocatalysts in green hydrogen industry. To address the dilemma of conventional crystalline-on-crystalline anti-chloride overlayer structures for seawater oxidation, a crystalline-amorphous CoS 2 -MnO x heterostructure is fabricated via precise deposition-order regulation. The amorphous MnO x underlayer not only exposes abundant active CoS 2 sites but also transports electron and ion flux to the surface for OER promotion and Cl − repulsion, establishing a novel and promising paradigm for durable seawater electrocatalysis. Download: Download high-res image (193KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lan Xie,Jiajia Hao,Yinsu Wu,Shengtao Xing
Non-radical activation of peroxymonosulfate (PMS) is a promising technology for removing refractory organic pollutants. However, improving its efficiency is still a challenge due to its ambiguous mechanism. In this work, amorphous MnO X was synthesized through the hydrothermal reaction between KMnO 4 and carbon nanopowder. The characterization results indicate that the hydrothermal temperature had little effect on the structure of the products but affected their surface composition. The sample prepared at 180 °C (MnO X -180) had rich oxygen vacancies and exhibited high activity for sulfamethoxazole (SMX) degradation with PMS. More than 97% of SMX was removed within 30 min by 0.5 g L −1 of MnO X -180 and 1 mmol L −1 of PMS at pH 0 = 6.5. Activated PMS adsorbed on catalyst surface and singlet oxygen ( 1 O 2 ) produced from the non-radical pathway were the active species. Surface Mn 4+ and oxygen vacancies were found to be responsible for the generation of activated PMS and 1 O 2 , respectively. The degradation efficiency of SMX by MnO X -180 increased with decreasing solution pH, which can be attributed to the enhanced production of activated PMS under acidic conditions. The water matrix had little effect on the performance of MnO X -180 due to the non-radical activation mechanism, suggesting its practical application in real water treatment.
研究领域:
环境科学
·
水处理技术
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Catalysis Science & Technology
·
2018
·Vol. 8
·期 6
·1621-1631
·
IF 5.365
Yuxi Gao,Xiaodong Wu,Robin Nord,Hanna Härelind,Duan Weng
The sulphur resistance and regeneration strategy of soot oxidation catalysts are critical to the application of catalytic diesel particulate filters (CDPFs). In the present work, Pt/MnOx–CeO2/Al2O3, Pt/Al2O3 and MnOx–CeO2/Al2O3 catalysts were sulphated and regenerated with ammonia. The soot oxidation activity of poisoned Pt/MnOx–CeO2/Al2O3 was recovered completely after 30 min reduction in 500 ppm NH3 at 550 °C. The amount, distribution and structure of sulphates were studied comprehensively for the sulphated and regenerated samples by thermogravimetric analysis (TGA), infrared (IR) spectroscopy, CO chemisorption and transmission electron microscopy (TEM). The NO oxidation of Pt catalysts was found to depend strongly on the particle size distribution, surface exposure and oxidation state of the precious metal. This, as well as the effect of the remaining surface sulphates, helped the regenerated catalysts achieve even higher catalytic activity for soot oxidation.
研究领域:
催化材料
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环境科学
·
化学工程
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Catalysts
·
2020
·Vol. 10
·期 6
·681
·
IF 3.52
Qian Zhang,Yiwen Jiang,Jingheng Gao,Mingli Fu,Sibei Zou,Yanxia Li,Daiqi Ye
A series of CeO2–MnOXcatalysts with different Ce contents was prepared using Mn–BTC MOF as a sacrificial template for toluene oxidation. Interestingly, the performance of CeO2–MnOXincreased rapidly only when the Ce content lower than 5%. The 1%-, 3%- and 10%-Ce-content samples exhibited the T90value of 325 °C, 291 °C and 277 °C, respectively. XRD shows that the catalyst phase changes significantly before (Mn3O4only) and after (Mn2O3, Mn3O4and CeO2) 3% Ce loading. All other results indicated that the Ce–Mn interface properties of different Ce content composite oxides was quite distinguishable in terms of removal and energy efficiency. XRD and XPS results further showed that there a Ce monolayer dispersion threshold existed on the interface of MnOX(3.2 wt%, confirmed by XPS), which caused the difference in performance increment. The dispersed Ce could be divided into a monolayer dispersion state (1–3%) and a crystalline phase state (>3%), according to the existence form, which corresponded to the significant and minor enhancements of toluene conversion rate. Importantly, the Ce in monolayer dispersion state obviously improved the redox properties of catalysts interface, while the Ce in crystal state not. The interfaces with monolayer dispersion Ce result in more abundant metal ion states, oxygen vacancies, better electron transfer performance and catalytic activity.
研究领域:
催化化学
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材料科学
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Advanced Science
·
2026
·
IF 14.1
Benzhi Wang,Ziyang Duan,Jeong Yeon Heo,Thu Ha Le,Byunggon Song,Sunhyeong Kwon,Ji Hoon Lee,Jonghwan Suhr,Hyung Mo Jeong
Electrocatalytic water splitting offers an efficient pathway for producing renewable hydrogen, which is considered a key strategy toward global carbon neutrality. Yet, under harsh industrial operating conditions, the catalyst inevitably undergoes dynamic structural reconstruction, oxidative dissolution of active sites, and mechanical detachment during high-potential anodic oxygen evolution reaction (OER), severely limiting their activity and stability. Here, we present an MnO x (composed of Mn 3 O 4 and Mn 2 O 3 ) layer on the FeCoNiCrMn high-entropy alloy (HEA) surface (denoted as HEA-ML) via laser powder bed fusion (LPBF) process and reveal that the MnO x layer suppresses multimetal dissolution in HEA and mitigates excessive surface reconstruction under OER conditions. Furthermore, the MnO x layer featuring a porous and rough surface enhances water adsorption and bubble diffusion, thereby accelerating interfacial mass transfer and OER kinetics. These outstanding features endow the catalyst to exhibit both excellent activity (227 ± 2 mV at 10 mA cm −2 ) and industrial-grade ultra-stable OER performance (operating stably for 1500 h at 1.0 A cm −2 ). Our research findings provide new insights into the structure-activity-stability relationship of HEA electrocatalysts and demonstrate a novel approach for designing industrially viable OER catalysts with high activity and ultra-stability.
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PubMed
高影响因子
Nature Communications
·
2026
·
IF 18.1
Zhao Yongqi,Wang Pu,Jiang Junjie,Zhao Ziwei,Xiu Aorui,Liu Xiaolong,Zhu Tingyu
Transition-metal oxides offer a low-cost alternative to precious metals for environmental catalysis, yet CO oxidation under humid and sulfur-laden conditions remains challenging due to rapid poisoning. Herein, we report an atomic dispersion of Ti‑decorated MnO x -Fe 2 O 3 catalyst that achieves high activity and remarkable H 2 O/SO 2 resistance. Atomically dispersed Ti provides electron-accepting 3d states from O 2p orbitals, which redistributes and stabilizes selected O 2p states while modifying their hybridization with neighboring Mn/Fe 3d orbitals. The localized electronic restructuring strengthens CO adsorption and facilitates lattice oxygen activation via a Mars-van Krevelen (MvK)-like mechanism, lowering the apparent activation energy to 64.59 kJ/mol. Simultaneously, Ti-O-Fe interfaces weaken SO 2 adsorption (from −1.96 eV to −0.19 eV) and suppress H 2 O competition, retaining >55% CO conversion under 10 vol% H 2 O and 10 ppm SO 2 , far surpassing the parent oxide (<10%). The orbital tuning strategy enables scalable poison resistant catalysts for industrial emission control, reducing reliance on precious‑metal systems.
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CHEMOSPHERE
·
2021
·
IF 7.086
Ziyang Xu,Shengpeng Mo,Yanxia Li,Yuchen Zhang,Junliang Wu,Mingli Fu,Xiaojun Niu,Yun Hu,Daiqi Ye
The problem of deep oxidation of low concentrations of VOCs in industrial tail gas is exceptionally urgent. The preparation of VOCs ozonation catalyst with a high mineralization rate is still a challenge. In this paper, manganese oxide carriers with different morphologies were synthesized by simple methods and used to catalyze ozone mineralization of toluene after loading Pt nanoparticles efficiently. The conversion of toluene over Pt/MnO x -T catalyst was more than 98 % at ambient temperature, and the mineralization rate of toluene was close to 100 % at 70 °C. Through a variety of characterization methods, the strong metal-support interaction (SMSI) between Pt nanoparticles and carriers was successfully constructed. It was found that SMSI successfully optimized the surface oxygen species and oxygen migration ability of the catalyst, and then realized the high degree of mineralization of toluene at low temperature. This paper guides the subsequent development of Pt–Mn catalysts for catalytic organic pollutants ozonation with high activity.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Lin-Cong He,Xu-Fang Wang,Chu-Feng Liu,Bei Li,Meng-Fei Luo,Jian Chen
An efficient MnO x /CeO 2 /ZSM-5 catalyst was developed for selective oxidation of diethylamine (DEA) with high N 2 selectivity in a wide temperature window ( Δ T = 140 °C), owing to the existence of oxidation and selective catalytic reduction (SCR) active sites. MnO x species prefer to locate on the surface of CeO 2 compared to ZSM-5, and the presence of CeO 2 is beneficial to form more Mn 4+ species, the active sites for oxidation reaction. The mechanistic investigation suggests that internal SCR of NO x generated from the over-oxidized DEA is the crucial pathway for N 2 generation. The high SCR activity of the MnO x /CeO 2 /ZSM-5 catalyst in oxidation conditions is mainly attributed to the synergistic catalysis of Mn 4+ species and acid sites of ZSM-5, the active sites for SCR reaction. Thus, it has been clearly clarified that addition of CeO 2 and its addition sequence could modulate the surface active sites of MnO x /ZSM-5 catalyst for the selective catalytic oxidation of DEA.
研究领域:
环境科学
·
催化化学
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Huayu Wu,Rongguan Lv,Rui Wang,Zhiyuan Zhao,Yuzhen Sun,Yu Liu,Yingna Chang,Jindi Wang,Kefan Song,Ming Chen,Rong Xing
3D Porous MnO x /rGO hydrogel (3DP MnO x /rGO hydrogel) as cathode material for aqueous zinc ion batteries (AZIBs) is synthesized by polyvinyl alcohol (PVA), nanowires of MnO x (NW MnO x ) and reduced graphene oxide (rGO) via repeated freeze-thaw method, which has a high flexibility and puncture resistance. The 3D self-supporting hydrogel presented complex 3D cross-linking system and excellent flexibility through hydrogen bonding and reinforcement of inorganic nano wires. The electrochemical and mechanical properties of the 3DP MnO x /rGO hydrogel are optimized by adjusting the respective percentages of NW MnO x (30%), rGO (5%), PVA (25%), and H 2 O (40%) in the total mass. The flexible hydrogel cathode exhibits a high capacity of 297.6 mA h g −1 and good cyclic stability after 500 cycles at 1 A g −1 . Finite element method confirms that the hydrogel material can alleviate the stress distribution caused by zincification process. The soft-packaged AZIBs, which utilize 3DP MnO x /rGO hydrogel as the cathode and Zn foil as the anode, exhibit excellent cycling performance (152.2 mA h g −1 at 1 A g −1 after 500 cycles under an angle of 180°) and provide a stable power supply across different bending angles.
研究领域:
材料科学
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电化学
·
能源存储
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yanping Yang,Shengchen Li,Shunli Shi,Jie Hu,Zexi Xuchen,Shunmin Ding,Dan zhao,Shengjun Deng,Weiming Xiao,Shuhua Wang,Chao Chen
Manganese oxide (MnO x ) catalysts are promising for low-temperature NH 3 -Selective Catalytic Reduction (NH 3 -SCR) with their superior catalytic performance. However, the presence of alkali metals in flue gases, particularly potassium (K), leads to catalyst deactivation and limits their industrial application. This study investigates the synergistic effects of Ce and Nb doping on the K resistance and low-temperature NH 3 -SCR activity of MnO x . The surface acidity and redox properties of MnO x were modulated by Ce and Nb modification. In addition, the phase structure, surface state and active sites of the catalysts were characterized before and after K poisoning. The results indicated that Nb 0.05 Ce 0.05 MnO x exhibited exceptional low-temperature performance, achieving over 90 % NO conversion at 125-250°C, along with significant resistance to K poisoning·NH 3 -TPD and in-situ experiments revealed that the loss of acid sites is the primary cause of K poisoning. The mechanism follows the L-H mechanism with L-acid sites as the main active sites on the catalyst surface and bridging nitrate as the key intermediate state. This research provides valuable insights into enhancing the industrial applicability of MnO x- based catalysts for low-temperature denitrification.
研究领域:
催化化学
·
环境工程
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高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Shixian Zhang,Chunming Xu,Rongzheng Ren,Jinshuo Qiao,Zhenhua Wang,Wang Sun,Kening Sun
As the demand for ethylene grows continuously in industry, conversion of ethane to ethylene has become more and more important; however, it still faces fundamental challenges of low ethane conversion, low ethylene selectivity, overoxidation, and instability of catalysts. Electrooxidative dehydrogenation of ethane (EODHE) in a solid oxide electrolysis cell (SOEC) is an alternative process. Here, a multiphase oxide Ce0.6Mn0.3Fe0.1O2−δ-NiFe-MnOx has been fabricated by a self-assembly process and utilized as the SOEC anode material for EODHE. The highest ethane conversions reached 52.23% with 94.11% ethylene selectivity at the anode side and CO with 10.9 mL min–1 cm–2 at the cathode side, at 1.8 V at 700 °C. The remarkable electrooxidative performance of CMF-NiFe-MnOx is ascribed to the NiFe alloy and MnOx nanoparticles and improvement of the concentration of oxygen vacancies within the fluorite substrate, generating dual active sites for C2H6 adsorption, dehydrogenation, and selective transformation of hydrogen without overoxidizing the ethylene generated. Such a tailored strategy achieves no significant degradation observed after 120 h of operation and constitutes a promising basis for EODHE.
研究领域:
材料科学
·
催化化学
·
能源转化
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PubMed
高影响因子
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