Catalysts
·
2026
·Vol. 16
·期 1
·
IF 4
Xin Liu,Jinshan Zhang,Tao Sun,Hisahiro Einaga,Hajime Hojo,Pengwei Huo
A series of novel Ce-modified MnCoAl layered double oxides (Ce/MCA LDOs) were prepared using solvothermal and impregnation methods for NH3-SCR denitration. Various characterizations, such as X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and H2temperature-programmed reduction (H2-TPR) were used to investigate their structural properties and the mechanism of ammonia selective catalytic reduction (NH3-SCR). The incorporation of Ce was found to effectively integrate into the LDO framework and enhance the catalytic activity over a wide temperature window. Moreover, the thermal stability and resistance of H2O and SO2were evaluated. In situ DRIFTS studies revealed that the reaction follows both the “Langmuir–Hinshelwood” (L–H) and “Eley–Rideal” (E–R) mechanisms. This work provides systematic insights into the design of LDO-based catalysts, demonstrating their potential for practical application in denitration.
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Journal of Central South University
·
2026
·Vol. 32
·期 11
·4248-4259
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IF 4.4
Wang Jia-yi,Liu Xin-li,Wu Zhuang-zhi,Wang De-zhi
Eco-friendly electrocatalytic nitrogen reduction reaction (NRR) is aimed to replace the traditional polluting industrial process, but NRR needs electrocatalysts with high selectivity and activity to boost desired NH 3 yield rate and Faradic efficiency (FE). In this work, high-entropy sulfides (HES) (FeCoNiMoM)S x (M=Cr, Cu, Mn) were synthesized via a two-step solvothermal method. The optimized composition for HES is (FeCoNiMoCr)S x , with promising NRR performance that NH 3 yield rate reached 47.97 µg/(h·mg cat ) at −0.7 V vs RHE and FE was 26.1% at −0.4 V vs RHE. Comprehensive characterization and electrochemical testing were performed to investigate the effects of the metal component on NRR performance. It reveals that (FeCoNiMoCr)S x shows more intense charge transport, more electrocatalytic active sites, higher selectivity, etc, resulting from the electron transport and element synergy of HES. Also, it is proved to have targeted NRR selectivity and limiting competitive hydrogen evolution reaction. The results offer promising guidance for further improving the NRR electrocatalysts based on transition elements.
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Applied Sciences-Basel
·
2018
·Vol. 8
·期 12
·
IF 1.689
Xinbo Zhu,Yaolin Wang,Yu Huang,Yuxiang Cai
In this work, a series of Ce-W-Ti catalysts were synthesized using a solution combustion method for the selective catalytic reduction (SCR) of NO with NH3at low temperatures. The reaction performance of NH3-SCR of NO was significantly improved over the Ce-W-Ti catalysts compared to Ce0.4Ti and W0.4Ti catalysts, while Ce0.2W0.2Ti showed the best activity among all the samples. The Ce0.2W0.2Ti catalyst exhibited over 90% removal of NO and 100% N2selectivity in the temperature range of 250–400 °C at a gas hourly space velocity (GHSV) of 120,000 mL·g−1·h−1. The Ce-W-Ti catalysts were characterized using N2adsorption-desorption, X-ray diffraction, X-ray photoelectron spectrometry and temperature programmed desorption of NH3to establish the structure-activity relationships of the Ce-W-Ti catalysts. The excellent catalytic performance of the Ce0.2W0.2Ti catalyst could be associated with the larger specific surface area, highly dispersed Ce and W species, increased amount of surface adsorbed oxygen (Oads) and enhanced total acidity on the catalyst surfaces.
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CATALYSIS TODAY
·
2020
·
IF 5.825
Jinfeng Han,Caixia Liu,Qingling Liu,Shuangchun Lu,Yalian Bi,Xiaohan Wang,Mingyu Guo,Chunfeng Song,Na Ji,Xuebin Lu,Degang Ma,Zhenguo Li
Novel Al-rich OFF-CHA twin-crystal zeolite was synthesized by one-pot hydrothermal method, and applied in ammonia-selective catalytic reduction (NH 3 -SCR) after copper ion exchange. Results indicated that Cu content in Cu-OFF-CHA played a significant role in NH 3 -SCR reaction. The insufficiency of copper activity sites and the formation of CuOx were the main reasons affecting low and high temperature SCR activity of catalyst, respectively. Cu 3.1 -OFF-CHA, with the optimal copper content, demonstrated over 90 % NOx conversion and exhibited excellent N 2 selectivity in the range from 160 to 550 ℃. Further research verified that the SCR activity of Cu 3.1 -OFF-CHA maintained above 80 % in the temperature range from 180–450 °C after hydrothermal treatment 16 h. The reason might be that Cu 2+ in Cu-OFF-CHA was migrated from CHA to OFF sites after hydrothermal treatment, and Cu 2+ in OFF sites on Cu-OFF-CHA was more stable, resulting in less conversion of the active site to CuOx clusters. Cu-OFF-CHA has the potential to be applied in SCR after-treatment systems of diesel exhaust due to the excellent SCR activity and hydrothermal stability.
研究领域:
催化化学
·
环境化学
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材料科学
·
化学工程
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 7
·2134-2141
·
IF 5
Lingling Li,Mingyuan Zhang,Tianhua Zhang,Yinglong Gao,Jun Ni,Yanliang Zhou,Jianxin Lin,Xiuyun Wang,Lilong Jiang
Ammonia (NH3) synthesis with hydrogen (H2) produced from renewable energy is a promising route to reduce carbon footprints and the dependence on fossil fuels. However, the development of highly efficient and stable catalyst for NH3 synthesis under mild conditions is a challenge. Herein, a series of boron nitride (BN)-supported Ru catalysts were synthesized, and the NH3 synthesis rate was enhanced significantly after the introduce of Ce. The developed RuCe2.4/BN catalyst with a Ce/Ru molar ratio of 2.4 exhibited the optimal NH3 synthesis rate of 14.6 mmolNH3 gcat−1 h−1 at 400 °C and 1.0 MPa, which was ∼21-fold that of the catalyst prepared without Ce. In situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption and X-ray photoemission spectroscopy coupled with electron energy loss spectroscopy revealed that the d–d electronic interaction between Ru and CeO2 can be differentially adjusted by a change in the Ce/Ru molar ratio. An appropriate amount of Ce could enhance the electronic interaction between the CeOy overlayer and Ru entities. Also, the CeOy overlayer acted as an “electron shuttle” and enhanced the charge transfer from Ce to the surface of Ru atoms. Finally, electron donation occurred from the surface abundancy of Ru atoms to N2 molecule through a d–π* interaction. Moreover, the introduction of excessive Ce could block Ru active sites, weaken the electron transfer and, therefore, decrease the NH3 synthesis rate.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Xiaoyue Chen,Songge Zhang,Xiu Qian,Zhangqian Liang,Yanjun Xue,Xiaoli Zhang,Jian Tian,Ye Han,Minhua Shao
Herein, we assemble semi-metallic 1T′ phase MoS 2 on the surface Ti 3 C 2 MXene (1T′-MoS 2 /Ti 3 C 2 composite) by one-step hydrothermal method for nitrogen fixation. 1T′-MoS 2 /Ti 3 C 2 composites present a high ammonia yield rate of 31.96 µg h −1 mg −1 cat. at − 0.95 V vs. RHE and a Faradaic efficiency (FE) of 30.75% at − 0.7 V, which is much better than pure 1T′-MoS 2 and pure Ti 3 C 2 MXenes alone. Furthermore, the 1T′-MoS 2 /Ti 3 C 2 composites exhibit good selectivity and stability with no significant decrease in ammonia yield rate and FE. Density functional theory (DFT) calculations reveal that 1T′-MoS 2 /Ti 3 C 2 composite makes the activation and further reduction of *N 2 more thermodynamically favorable than pure 1T′-MoS 2 . 1 5 N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N 2 in the electrolyte.
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FUEL
·
2022
·
IF 8.035
Yiqing Zeng,Weilong Rong,Shule Zhang,Yanan Wang,Qin Zhong
Ammonia selective catalytic reduction (NH 3 -SCR) technique for nitrogen oxide (NO x ) elimination of low temperature flue gas (<200 °C) requires huge energy consumption and operation costs. In this work, a CuO modified V 2 O 5 -WO 3 /TiO 2 (Cu/VWTi) catalyst are constructed to achieve the aim of enhancing the temperature of flue gas via using the heat released by CO oxidation, thereby promoting the NH 3 -SCR of NO x reaction. Benefiting from the synergistic effect between CuO and VWTi in the adsorption and activation of reactants, Cu/VWTi catalyst shows high NO x (>90%) and CO (>90%) removal efficiency at the temperature range of 225–270 °C and a GHSV of 40,000 h −1 . Moreover, it is found that the completely oxidation of 2000 ppm CO can increase the flue gas temperature by about 20 °C. Therefore, developing catalyst that can achieve simultaneously NH 3 -SCR of NO x and CO oxidation is a feasible method to deduce the energy consumption and operation costs of NH 3 -SCR of NO x system in low temperature flue gas. Finally, the reaction process and SO 2 deactivation effect over Cu/VWTi catalyst was studied via in-situ DRIFT. This work might provide some guidance for the design of catalysts to eliminate multiple pollutants.
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AICHE JOURNAL
·
2022
·Vol. 68
·期 11
·e17834
·
IF 4.167
Wuyuan Liu,Zhaoying Wang,Ming Sun,Jiajian Gao,Lifeng Wang,Zihan Gao,Yingying Xu,Xiangyun Zhao,Cheng Zhang,Lin Yu
A series of CeO 2 modified Cu-SSZ-13 monolith catalysts were prepared by embedding CeO 2 into the washcoat of Cu-SSZ-13 monolith catalyst through solvent combustion method. These CexCu-SSZ-13 catalysts were studied in the selective catalytic reduction (SCR) of NO with NH 3 , among which the Ce2Cu-SSZ-13 catalyst exhibited the best low-temperature activity, hydrothermal stability, and sulfur resistance. The physicochemical properties of the catalysts were characterized using multiple methods. Results showed that the acidity, redox capacity, and ammonia adsorption capacity significantly enhanced after CeO 2 modification, thus leading to the high performance of Ce2Cu-SSZ-13 catalyst. Furthermore, the introduction of CeO 2 induced the fast SCR reaction by promoting the oxidation of NO to NO 2 . Analog calculation suggested that the porous structure generated via solvent combustion in the washcoat effectively increased the diffusion rate of reaction. In situ diffuse reflectance infrared Fourier transform spectroscopy ( in situ DRIFT) analysis showed that Brønsted acid sites were the main active center and the reaction followed Eley–Rideal mechanism.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 35
·16743-16751
·
IF 3.925
Kun Jiang,Kai Li,Shuirong Li,Yan Li,Tao Li,Yun-Quan Liu,Duo Wang,Yueyuan Ye
Transition metal nitrogenous complexes have been extensively studied for electrochemical synthesis of ammonia due to their great capabilities in adsorbing and activating nitrogen molecules; yet the improvement of their catalytic performance is still a big challenge. Herein, a series of novel bimetallic Fe, Mo–N nanosheet arrays (FeMo–N) supported on nickel foam were fabricated through a facile hydrothermal–pyrolysis method, which were used as electrocatalysts for the nitrogen reduction reaction (NRR). It was discovered that the catalyst Fe1Mo1–N exhibited a promising performance with a NH3 yield rate of 46.64 μg mg−1cat. h−1 and a faradaic efficiency (FE) of 1.12% at −0.8 V vs. RHE, which also demonstrated excellent selectivity and thermal stability. The specific two-dimensional nanosheet morphology of the catalyst was believed to be the major reason contributing to the prominent electrochemical performance. The XPS characterization and NH3 yield study at different N contents in the M–N bond further revealed that FeMo–N species are the primary active centers for the NRR, and the N content forming the M–N bond is closely related to the catalytic activity.
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International Journal of Refrigeration
·
2021
·
IF 3.629
Zhenghao Jin,Shuhong Li,Runfa Zhou,Mengkai Xu,Weixue Jiang,Kai Du
The newly NH 3 – H 2 O – LiBr working fluid can decrease the power wasted in the generator, thus improves the COP of the ammonia absorption refrigeration system. But the applying of NH 3 – H 2 O – LiBr working fluid decreases the ammonia absorption efficiency, so the COP of the system is still unsatisfactory. To further enhance the COP of the NH 3 – H 2 O - LiBr absorption refrigeration system, TiO 2 nanoparticles are added to the NH 3 – H 2 O - LiBr working fluid in this study. And the effects of TiO 2 nanoparticles concentration on the performances of the generator, absorber, evaporator, condenser, and solution heat exchanger are tested in an ARS experimental system. The experimental results indicate that the addition of TiO 2 nanoparticles increases the P g , P e , P a , and P c , meaning that the value of ammonia produced in the generator increases. Therefore, the COP and iCOP of the system are improved by adding TiO 2 nanoparticles, and the COP is maximum improved by 18.96% compared with the ammonia-water absorption refrigeration system. When the x TiO2 is increased from 0.3% to 0.5%, the increase rate of the COP decreases because the newly added nanoparticles do not disperse well. So 0.3% is a better choice for the TiO 2 nanoparticles concentration when comprehensively considering the dispersion stability of nanoparticles and the COP.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Li Luo,Jiaran Li,Xiaoyan Chen,Xuegong Cao,Yibang Liu,Zhixin Wu,Xiaoyan Luo,Congmin Wang
In this work, porous PIL-TAs were reported for superhigh capacity and reversible NH 3 uptake, where PIL-TAs are cobaltous thiocyanate (Co(II)(SCN) 4 2- , TA) functionalized poly ionic liquids (PILs). Due to the structural support of TA as well as the interactions between TA and imidazolium cation, the PIL-TAs possess porous structure and optimized properties. Superhigh NH 3 uptake capacity of 13.2–20.1 mmol g −1 at STP of PIL-TAs was achieved, which is higher than most of the reported sorbents. In detail, the cooperative interactions including the NH 3 coordinating with Co(II) instead of SCN - and hydrogen bonding of C2H in imidazolium (C2H…NH 3 ) benefit to high capacity of NH 3 uptake. Reversely, the NH 3 release would be directed by the competition of the free SCN - with NH 3 to reform PIL-TAs. The competitive interaction with SCN - promotes NH 3 release by temperature and pressure swinging, which contributes the adsorbents recyclable. The cooperative and competitive interactions make these PIL-TAs possess high gas capacity and feasible desorption, which might be a potential strategy for designing novel gas sorbents.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 15
·5125-5134
·
IF 6.119
Yanke Yu,Xianfang Yi,Jiali Zhang,Zhaojian Tong,Changwei Chen,Mudi Ma,Chi He,Jinxiu Wang,Jinsheng Chen,Bingbing Chen
Non-vanadium-based catalysts with high SO2 tolerance are still interesting in selective catalytic reduction of NO by NH3 (NH3-SCR) and SO2 adsorption is the foremost step for the deactivation of catalysts. In order to alleviate the adsorption of SO2, we fabricated a series of rhenium (Re; without stable sulfate) supported TiO2 catalysts and studied their SO2 tolerance for the first time. Owing to suitable surface acidity and reducibility, ReOx/TiO2 catalysts exhibited satisfactory activity in a wide temperature range of 250–350 °C. As expected, experimental results and DFT calculations indicated that SO2 adsorption on ReOx/TiO2 catalysts was rather weak, thus the catalysts performed excellent SO2 tolerance in the NH3-SCR reaction. Moreover, in situ DRIFTS indicated that the NH3-SCR reaction on ReOx/TiO2 catalysts followed the Eley–Rideal mechanism and SO2 had little effect on the reaction mechanism. Our findings should provide new insights into the development of SCR catalysts with high SO2 tolerance.
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