ACS ES&T Engineering
·
2026
·
IF 6.3
Xu Pan,Jiangkun Xie,Mingze Jiao,Liang Shan,Hongyuan Qi,Wenjun Huang,Zan Qu,Naiqiang Yan,Haomiao Xu
Methane selective catalytic reduction (CH4-SCR) represents a promising strategy for nitrogen oxides (NOx) abatement, yet its practical application is hindered by catalyst deactivation in the presence of water, caused by competitive adsorption on acid sites and irreversible hydroxylation of active metal species. In this study, we developed a dual-functional In@H-Beta/Fe2O3 catalyst through sequential ion-exchange and impregnation. This architecture confines indium species within the channels of H-Beta zeolite, while Fe2O3 nanoparticles are dispersed on the external surface, creating a synergistic system featuring a hydrophobic layer and strong Fe–O–In interfacial interactions. Under 5% H2O conditions, the optimized catalyst achieves 85% NOx conversion (vs 40% for conventional In@H-Beta). The enhanced water resistance is attributed to two factors: first, Fe2O3 establishes a physical barrier that protects acid sites and stabilizes InO+ active sites via Fe–O–In bonding, thereby inhibiting hydroxylation; second, strong interfacial Fe–O–In interactions further stabilize InO+ active sites against aqueous deactivation. Additionally, the Fe2+/Fe3+ redox cycle is proposed to facilitate O2 activation. In situ DRIFTS studies under 5% H2O confirm effective CH4 activation, as indicated by markedly more intense C–H stretching bands compared with In@H-Beta. The reaction pathway involves NO activation over Brønsted acid sites to form nitrate species, and CH4 activation on InO+ sites generating methyl radicals, which subsequently participate in NOx reduction. This work offers a new design strategy for developing highly active and water-tolerant CH4-SCR catalysts suitable for industrial flue gas treatment.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Fan Yao,Ang Cao,Bing Zhou,Shengyong Lu,Jianhua Yan,Damien Debecher,Yaqi Peng
The synergistic removal of NO and chlorinated volatile organic compounds (CVOCs) using bifunctional catalysts has emerged as a cutting-edge strategy in environmental catalysis. However, achieving both efficient NOx selective catalytic reduction and CVOCs catalytic oxidation remains fundamentally challenging due to the inherent trade-off between activity and selectivity. Herein, we demonstrate that this trade-off can be overcome by applying a mechanochemical strategy coupled with electronic band modulation to construct a novel heterojunction catalyst, in which MnCe oxides are integrated with and piezoelectric BaTiO 3 to form a heterojunction interface. The optimized TB-MnCe catalyst exhibits remarkable synergistic performance, achieving the synergistic removal of o-dichlorobenzene (>80%) and NOx (100%) within a broad temperature range of 250–350 °C. Combined experimental and theoretical investigations reveal an interfacial charge transfer of approximately 4.6 electrons from BaTiO 3 to MnCe during mechanochemical treatment. This charge redistribution, mediated by the engineered interface, significantly enhances the redox capability of the active sites and promotes cooperative reactions. This work highlights that atomic-level interfacial electronic modulation induced by mechanochemical processing provides a powerful route to resolve the activity-selectivity dilemma in bifunctional catalysis. Download: Download high-res image (128KB) Download: Download full-size image
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PubMed
高影响因子
MOLECULES
·
2025
·Vol. 30
·期 13
·2691
·
IF 4.6
Jiuhu Zhao,Jingjing Jiang,Guanyu Chen,Meng Wang,Xiaoyuan Zuo,Yanjiao Bi,Rongshu Zhu
The selective catalytic reduction of NOxwith CH4(CH4-SCR) holds the potential to simultaneously abate harmful NOxand CH4greenhouse gases. In this study, a series of bimetallic M-In/H-SSZ-39 catalysts (where M represents Cr, Co, Ce, and Fe) were prepared via an ion exchange method and subsequently evaluated for their CH4-SCR activity. The influences of the preparation parameters, including the metal ion concentration and calcination temperature, as well as the operating conditions, such as the CH4/NO ratio, O2concentration, water vapor content, and gas hourly space velocity (GHSV), on the catalytic activity of the optimal Cr-In/H-SSZ-39 catalyst were meticulously examined. The results revealed that the Cr-In/H-SSZ-39 catalyst exhibited peak CH4-SCR catalytic performance when the Cr(NO3)3concentration was 0.0075 M, the In(NO3)3concentration was 0.066 M, and the calcination temperature was 500 °C. Under optimal operating conditions, namely GHSV of 10,000 h−1, 400 ppm NO, 800 ppm CH4, 15 vol% O2, and 6 vol% H2O, the NOxconversion rate reached 93.4%. To shed light on the excellent performance of Cr-In/H-SSZ-39 under humid conditions, a comparative analysis of the crystalline phase, chemical composition, pore structure, surface chemical state, surface acidity, and redox properties of Cr-In/H-SSZ-39 and In/H-SSZ-39 was conducted. The characterization results indicated that the incorporation of Cr into In/H-SSZ-39 enhanced its acidity and also facilitated the generation of InO+active species, which promoted the oxidation of NO and the activation of CH4, respectively. A synergistic effect was observed between Cr and In species, which significantly improved the redox properties of the catalyst. Consequently, the activated CH4could further interact with InO+to produce carbon-containing intermediates such as HCOO−, which ultimately reacted with nitrate-based intermediates to yield N2, CO2, and H2O.
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PubMed
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Liu Wei,Lv Yang,Ou Honghui,Zhang Jiqiu,Ren Yuxi,Xia Mengyang,Li Yang,Li He,Ren Xiaoling,Hu Huagui,Yang Guidong
Plasma-electrochemical tandem conversion with NO x − as intermediates promises a route for renewable ammonia (NH 3 ) synthesis from air and water. However, a critical challenge lies in developing electrolyzers capable of operating efficiently at large current densities. Here, we present a scalable membrane electrode assembly electrolyzer with a full runner design (MEA-FR) that achieves efficient NH 3 production at industrial current densities. Compared to conventional serpentine runner configuration, MEA-FR leveraging forced convection within porous electrodes achieves three-order-of-magnitude enhancement in NO x − mass transfer flux. This design, meanwhile, generates strong shear forces across the porous electrode, promoting rapid detachment of O 2 bubbles at the anode and reducing overpotential losses. Notably, MEA-FR exhibits a high Faradaic efficiency of 91.8 ± 1.4% for NH 3 synthesis at 500 mA cm −2 , significantly outperforming the serpentine runner counterparts (64.9 ± 1.1%). Furthermore, a scaled-up 4 × 25 cm 2 MEA-FR stack with four modular cells is assembled with rotationally symmetric bipolar plates, delivering high NO x − conversion efficiency (>95%), high Faradaic efficiency (>91%), and long-term stability (>200 h) under industrial-relevant current densities.
研究领域:
电化学
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可再生能源
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氨合成
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化学工程
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材料科学
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环境技术
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Rui Li,Xiangqiong Jiang,Jiecheng Lin,Zhiping Zhang,Qintong Huang,Guangying Fu,Yujun Zhu,Jiuxing Jiang
SSZ-16 zeolite with AFX topology was synthesized by hydrothermal method using 1,4-diazabicyclo[2.2.2]-octane-C4-diquat dibromide as organic structure directing agent. Cu x -SSZ-16 catalysts were prepared by exchanging SSZ-16 zeolite with Cu and applied for selective catalytic reduction (SCR) of NO x with ammonia. Among these catalysts, Cu 2.2 -SSZ-16 performs the best SCR denitration (deNO x ) performance that above 90% NO x conversion can be achieved at 175–600 °C. Especially, the influences of the hydrothermal aging at various temperatures (650, 750 and 850 °C) on active species and AFX framework of the Cu 2.2 -SSZ-16 catalyst are investigated in detail by various characterization methods including XRD, SEM , H 2 -TPR, NMR, UV–vis-DRS, EPR, NH 3 -TPD and in situ DRIFTS . Cu 2.2 -SSZ-16 still shows good NH 3 -SCR activity after hydrothermal aging at 650 and 750 °C due to more Cu 2+ -2Z species in the sample. Still, obvious deactivation can be observed after hydrothermal aging at 850 °C because of the collapse of AFX skeleton and the weak interaction between active Cu species and the skeleton. Nevertheless, Cu 2.2 -SSZ-16 is a competitive candidate for NH 3 -SCR deNO x reaction in practical applications.
研究领域:
催化化学
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环境科学
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高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2017
·
IF 4.217
Shu-ming Liu,Rui-tang Guo,Shu-xian Wang,Wei-guo Pan,Peng Sun,Ming-yuan Li,Shuai-wei Liu
Ca salts in fly ash have a deactivation effect on SCR catalyst. In this study, the deactivation mechanism of Ca on Ce/TiO 2 catalyst was investigated in term of the in situ DRIFT study. The experimental results indicate that the poisoning effect increases with reaction temperature. From the results of in situ DRIFT study, it may be concluded that the NH 3 -SCR reaction over Ce/TiO 2 catalyst takes place though two pathways: the L -H mechanisms (<200 °C) and the E-R mechanism (>200 °C). For Ce/TiO 2 -Ca, the NH 3 -SCR reaction over it is mainly controlled by L -H mechanism. The deactivation of Ce/TiO 2 -Ca lies in the following two aspects: (1) the inhibited NH 3 adsorption and NO oxidation (<200 °C); (2) the greatly suppressed NH 3 adsorption and activation (>200 °C).
研究领域:
环境催化
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化学工程
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大气污染控制
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材料科学
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高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2026
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IF 6.2
Jiangtao Meng,Haobo Chang,Lei Ren,Jingkuan Li,Jing Wang
Pyrolysis conversion of sewage sludge faces a technical bottleneck of NOx pollution caused by high ash content and rich protein components. Among them, the influence of CaO on nitrogen transformation during amino acid pyrolysis is significant, yet the underlying principles and mechanisms governing its effect across amino acid with different structures remain poorly understood. To address this issue, this study focused on four representative amino acids: leucine (Leu), aspartic acid (Asp), phenylalanine (Phe), and histidine (His). It systematically investigated the migration behavior of nitrogen during their pyrolysis, which was driven by the synergistic effects of temperature and CaO. The results demonstrated that CaO reconstructed the directional migration pathways of nitrogen into char, tar, and gas. This reconstruction is achieved through four key actions: complexation, alkaline deamination, hydrolysis, and CO 2 mineralization. This reconstruction exhibits a decisive structural dependency: In polar amino acids (Asp, His), CaO strongly complexes with carboxyl/imidazole groups at low temperatures (255 ℃ and 350 ℃). This interaction traps nitrogen intermediates and diverts them toward stable structures in char, such as nitrile-N and CaCxNy. Consequently, the formation of gas-phase NOx precursors is suppressed. In contrast, for non-polar amino acids (Leu, Phe), CaO’s alkaline effect dominates, enhancing early deamination to release NH 3 and promoting nitrogen migration via the isocyanic acid pathway, which increases nitrogen allocation to the gas phase. This study has revealed the pathway reconstruction mechanism and structural response patterns of nitrogen migration during pyrolysis under CaO influence. It further proposed design strategies for the directional regulation of nitrogen, thereby providing fundamental support and a mechanistic guide for achieving low-NOx pyrolysis and the conversion of N-rich biomass into the zero-carbon fuel, NH 3 .
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高影响因子
ACS Applied Materials & Interfaces
·
2014
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IF 5.9
Lei Chen,Zhichun Si,Xiaodong Wu,Duan Weng
A CuO–CeO2–TiO2 catalyst for selective catalytic reduction of NOx with NH3 (NH3-SCR) at low temperatures was prepared by a sol–gel method and characterized by X-ray diffraction, Brunner–Emmett–Teller surface area, ultraviolet–visible spectroscopy, H2 temperature-programmed reduction, scanning electron microscopy and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS). The CuO–CeO2–TiO2 ternary oxide catalyst shows excellent NH3-SCR activity in a low-temperature range of 150–250 °C. Lewis acid sites generated from Cu2+ are the main active sites for ammonia activation at low temperature, which is crucial for low temperature NH3-SCR activity. The introduction of ceria results in increased reducibility of CuO species and strong interactions between CuO particles with the matrix. The interactions between copper, cerium and titanium oxides lead to high dispersion of metal oxides with increased active oxygen and enhanced catalyst acidity. Homogeneously mixed metal oxides facilitate the “fast SCR” reaction among Cu2+–NO, nitrate (coordinated on cerium sites) and ammonia (on titanium sites) on the CuO–CeO2–TiO2 catalyst at low temperatures.
研究领域:
环境催化
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材料化学
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表面科学
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化学工程
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大气污染控制
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高影响因子
Journal of Cleaner Production
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2021
·
IF 9.297
Yu Yang,Tao Ji,Yuan Lin,Wenyue Su
Photocatalytic cementitious materials (PCMs) are a promising material for air purification at ambient conditions. Herein, polymeric carbon nitride (PCN), a material with high chemical and thermal stability that is responsive to visible light, was employed for the fabrication of PCMs with the assistance of two adhesives (i.e., acrylic latex and waterglass). The effect of the adhesives on the photocatalytic removal of nitrogen oxides (NO x ) and their stability over the PCN-coated PCMs was studied under various environmental conditions. Experimental results indicated that the waterglass-based PCMs outperformed the acrylic latex-based PCMs in terms of the photocatalytic NO x removal under visible light irradiation and stability in the peeling and washing trials. The relative humidity had beneficial effects on the NO x removal efficiency for the acrylic latex and deleterious effects on the waterglass incorporated PCMs, due to their distinct surface wettability . The ambient temperature, initial nitrogen monoxide (NO) concentration, and light intensity had a positive impact on the NO x removal efficiency for the as-prepared PCMs.
研究领域:
材料科学
·
环境科学
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DOI
高影响因子
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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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yiqing Zeng,Yanan Wang,Plaifa Hongmanorom,Zhigang Wang,Shule Zhang,Jiatang Chen,Qin Zhong,Sibudjing Kawi
Highly-efficient CeO 2 -TiO 2 -based catalyst is an attractive alternative to traditional V 2 O 5 -based catalysts for selective catalytic reduction of NO x by NH 3 (NH 3 -SCR). Herein, we construct an efficient and stable P-doped CeO 2 /TiO 2 ( y CeTi-P x ) catalyst by dispersing CeO 2 on strongly acidic and highly stable mesoporous P-doped TiO 2 (Ti-P x ). The characteristic structure of Ti-P x causes highly dispersed CeO 2 , strong active component-support interaction, and abundant surface active oxygen and acid sites on CeTi-P catalyst. Therefore, y CeTi-P x catalyst exhibits much higher catalytic activity than y CeTi catalyst at temperature of 200–450 °C. The y CeTi-P x catalysts show high activity in the presence of H 2 O and strong resistance to H 2 O + SO 2 at medium-high temperature, implying that they have great industrial application prospects. Different P/Ti ratio and CeO 2 loading content were investigated. Excessive P doping can block the Ce 4+ /Ce 3+ redox couple, and suppress redox sites on y CeTi-P x catalyst. Additionally, increasing CeO 2 content can reduce the NH 3 capacity of y CeTi-P x catalyst. By controlling the P/Ti ratio and CeO 2 loading content, surface acid sites and redox sites on y CeTi-P x catalyst can be balanced to obtain the best catalytic activity. This work demonstrates a feasible method in adjusting acid sites and redox sites on CeTi catalyst, which ultimately contributes to the new design of CeO 2 -TiO 2 -based catalyst.
研究领域:
环境科学
·
催化化学
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高影响因子
JOURNAL OF RARE EARTHS
·
2019
·
IF 2.846
Lei Chen,Ding Wang,Jiadao Wang,Duan Weng,Li Cao
The CeO 2 -TiO 2 (CeTi) and CeO 2 /WO 3 -TiO 2 (CeWTi) catalysts were prepared by sol-gel method. The as-prepared catalysts were hydrothermally treated at 760 °C for 48 h in air containing 10 vol% H 2 O to obtain the hydrothermal aged catalysts. The sulfur aged catalysts were treated at 400 °C with 100 ppm SO 2 , 10% water vapor, air balance for 48 h and catalysts. The powder X-ray diffraction (XRD) and Raman results indicate that the crystallization of hydrothermal aged catalysts is more serious than sulfur aged catalysts. In addition, tungsten species can stabilize the CeTi catalyst from grain growth. According to the results of in situ diffuse reflectance infrared Fourier transform spectra (DRIFTS), temperature-programmed desorption of ammonia (NH 3 -TPD), H 2 temperature-programmed reduction (H 2 -TPR) and ammonia oxidation , the aging process leads to loss of surface area, redox properties, surface acidities and surface ceria concentration, especially for the hydrothermal aging. The NH 3 -NO/NO 2 SCR performances of sulfur aged catalysts are better than that of hydrothermal aged catalysts. Compared with CeTi catalyst, the addition of tungsten inhibits the crystallization of catalyst. So that more acid sites and active sites are retained. This is also the reason why tungsten addition improves the NH 3 -NO/NO 2 SCR performance of CeTi catalyst.
研究领域:
催化化学
·
环境科学
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高影响因子
危险品化学品经营许可证（带存储）