CATALYSIS COMMUNICATIONS
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2022
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IF 3.51
Bin Chen,Jian Qiu,Liang Xu,Yan Cui
The Ni/Ce 0.8 Zr 0.2 O 2 catalysts with different Ni doping amounts (5 wt%, 10 wt%, 15 wt%, 20 wt%, and 25 wt%) are prepared by the impregnation technique and used as CO 2 methanation catalysts in this work. The effects of various Ni doping loading on CO 2 methanation catalytic performance at low temperatures were investigated in this catalytic system. The results show that the catalyst with 15 wt% Ni doping shows the best catalytic performance. Since the heated sintering of Ni nanoparticles was prevented efficiently by CO 2 methanation, these mesoporous catalysts exhibit excellent stability. Therefore, the catalyst is expected to be an efficient CO 2 methanation catalyst at low temperatures.
研究领域:
催化
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环境化学
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材料科学
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产品关联
DOI
高影响因子
Journal of CO2 Utilization
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2019
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IF 5.189
Haoxi Jiang,Qiang Gao,Shutian Wang,Yifei Chen,Minhua Zhang
Carbon dioxide methanation is of great importance for both environment and energy because of the reduction of carbon dioxide emissions and the utilization of carbon source. In this work, UiO-66 was employed as the support for palladium nanoparticles via a sol-gel method to enhance the activity of CO 2 methanation. The physical-chemical properties of as-prepared catalysts were characterized using N 2 adsorption-desorption, X-ray diffraction (XRD), transmission electron microscope (TEM), temperature programmed desorption (TPD), temperature programmed reduction (TPR), thermo-gravimetric analysis (TGA), Fourier-transform infrared (FTIR) spectroscopy and X-ray photoelectron spectroscopy (XPS). It was found that there was a synergistic effect between UiO-66 and supported Pd. CO 2 could be activated in UiO-66 via its Zr 6 O 4 (OH) 4 nods, while H 2 molecules were dissociated at Pd for further hydrogenation of activated CO 2 . As a result, the catalyst with a Pd loading of 6 wt.% exhibited a high activity with 56.0% of CO 2 conversion and 97.3% of CH 4 selectivity, corresponding to a STY of 856 g·h −1 ·kg cat −1 at 4 MPa and 340 °C.
研究领域:
环境科学
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能源化学
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产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
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2024
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IF 7.2
Yucan He,Dongsen Mao,Qiangsheng Guo,Jun Yu
A series of highly ordered microporous Ce-based metal-organic frameworks (MOFs) were synthesized as the precursors for catalyst construction. The corresponding Ru catalysts were prepared by Ru impregnation on the derived CeO 2 by pyrolysis of Ce-MOF, and investigated for the CH 4 synthesis via CO 2 hydrogenation. Among the catalysts, Ru catalyst supported on the CeO 2 -B derived from Ce-BDC exhibited a highly competitive efficiency for CO 2 methanation, giving a CH 4 selectivity of 100% with a CO 2 conversion of 62% at 275 °C and 0.1 MPa, and the CH 4 productivity reached 0.49 mol/(mol Ru ·h). Characterization results revealed that more oxygen vacancies and corresponding surface oxygen species formed on the surface of CeO 2 -B derived from Ce-BDC caused to the stronger interaction between Ru and CeO 2 -B, which promoted the CO 2 adsorption and hydrogenation capacity of the catalyst, resulting in its better catalytic property. In situ diffuse reflectance infrared Fourier transform (DRIFT) studies further revealed that the route of HCOO* into CH 4 is a more competitive way of CO 2 hydrogenation to CH 4 .
研究领域:
化学工程
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催化材料
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yajing Hu,Yong Men,Shuyi Xu,Yuanfen Feng,Jinguo Wang,Kaijie Liu,Yibo Zhang
Constructing the interface of Ni/Y 2 O 3 heterogeneous catalyst is a feasible strategy for efficient catalyst design in CO 2 methanation, which can create the active Y–O–Ni interfacial sites by utilizing the interaction between Ni and Y 2 O 3 . In this work, the strategy of using different nickel precursors (nickel nitrate, nickel acetate, basic nickel carbonate and nickel citrate) was used to prepare various Ni-based catalysts supported on Y 2 O 3 , which were estimated for their catalytic performance on CO 2 methanation. The catalysts were characterized based on BET, XRD, TEM, H 2 -TPR, XPS and CO 2 -TPD, etc. The results indicated a close correlation between the metal dispersion and particle size of Ni/Y 2 O 3 catalysts and the nickel precursor employed. The Y–O–Ni interface structure in Ni/Y 2 O 3 catalysts, associated with basic sites, provides a richer source of basic sites, offering more active sites for CO 2 adsorption and activation. Ni/Y 2 O 3 catalyst prepared with nickel nitrate as the precursor exhibited characteristics such as a highly enhanced nickel dispersion, a smaller nickel particle size, and more abundant metallic Ni 0 sites. Moreover, nickel nitrate-derived Ni/Y 2 O 3 catalyst exhibited optimal catalytic activity, achieving a CO 2 conversion rate of up to 92 % at 300 °C, with 100 % selectivity to CH 4 , and displaying good stability over 30 h. Therefore, the dispersion of Ni and the size of Ni particles could be controlled by adjusting the precursor, which is closely associated with the catalytic activity of Ni/Y 2 O 3 catalyst. This work unveils the interface-property relationship of Ni/Y 2 O 3 catalysts and provides a new insight into strategy of constructing more effective Ni-based catalyst for CO 2 methanation through the controlled nickel precursor.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2022
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IF 0.847
Zheyue Li,Di Wu,Wanbing Gong,Jiayi Li,Shuaikang Sang,Hengjie Liu,Ran Long,Yujie Xiong
Solar-driven CO 2 methanation is an imperative and promising approach to relieve the global warming and environmental crisis, yet remains a great challenge due to the low reaction efficiency, unsatisfactory selectivity and poor stability. In this work, we demonstrate a facile and efficient strategy to prepare Ru-doped TiO 2 photocatalyst with tunable oxygen vacancies using the ascorbic acid as a reducing agent for the CO 2 methanation reaction. The optimal Ru-TiO 2 -OV-50 exhibits a remarkable CH 4 production rate of 81.7 mmol g −1 h −1 with a 100% CH 4 selectivity under a 1.5 W cm −2 light illumination, which is significantly higher than commercial Ru/TiO 2 and other reported catalysts. We reveal that the superior photocatalytic CO 2 methanation performance is mainly due to the synergistic effect of Ru doping and TiO 2 with tunable oxygen vacancies. Impressively, the light rather than thermal effect is confirmed as the main influencing factor by experimental studies. In addition, in situ spectroscopic technology is performed to investigate the CO 2 methanation reaction pathway. This work will open an avenue to design and prepare highly efficient photocatalyst with tunable oxygen vacancies for CO 2 conversion and other related applications.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2025
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IF 6.5
Wenhao Zhang,Liang shen,Longhao Xu,Fayang Zhou,Fengyin Sun,Jing Xu,Minghui Zhu
Hydrogenation of CO 2 to methane is a feasible solution to the growing global environmental and energy challenges. Nickel-based catalysts are efficient and cost effective for CO 2 methanation. Hernin, we synthesized Mn-promoted Ni/Al 2 O 3 catalysts with facilitated CO 2 methanation and elucidated the crucial role of Mn. After Mn doping, NiMn/Al 2 O 3 catalysts showed improved NiO dispersion. Subsequently, H 2 reduction and CO 2 methanation treatments resulted in reduction of NiO and MnO 2 into Ni and MnO, and incorporation of Ni 2+ into MnO lattice, forming NiMnO x and creating numerous Ni-NiMnO x interfaces. The abundant oxygen vacancies from NiMnO x could enhance CO 2 activation. Moreover, oxygen vacancies at the interface also promote electron transfer from Ni and MnO, leading to electron-poor Ni nanoparticles and thus significantly promoting the *CO methanation. Ultimately, the electron-poor Ni nanoparticles and abundant oxygen vacancies at the Ni-NiMnO x interface jointly facilitate CO 2 methanation.
研究领域:
催化化学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
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2021
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IF 9.676
Qiaojuan Wang,Yating Gao,Chantsalmaa Tumurbaatar,Tungalagtamir Bold,Fei Wei,Yihu Dai,Yanhui Yang
Carbonate-modified metal-support interfaces allow Ru/MnCO 3 catalyst to exhibit over 99% selectivity, great specific activity and long-term anti-CO poisoning stability in atmospheric CO 2 methanation. As a contrast, Ru/MnO catalyst with metal-oxide interfaces prefers reverse water–gas shift rather than methanation route, along with a remarkably lower activity and a less than 15% CH 4 selectivity. The carbonate-modified interfaces are found to stabilize the Ru species and activate CO 2 and H 2 molecules. Ru-CO* species are identified as the reaction intermediates steadily formed from CO 2 dissociation, which show moderate adsorption strength and high reactivity in further hydrogenation to CH 4 . Furthermore, carbonates of Ru/MnCO 3 are found to be consumed by hydrogenation to form CH 4 and replenished by exchange with CO 2 , which are in a dynamic equilibrium during the reaction. Modification with surface carbonates is proved as an efficient strategy to endow metal-support interfaces of Ru-based catalysts with unique catalytic functions for selective CO 2 hydrogenation.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
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2017
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IF 2.594
Jinwei Sun,Yujiang Wang,Haikui Zou,Xiaoguang Guo,Zhou-jun Wang
Nanosheet (S) and nanoplate (P) γ-Al 2 O 3 were synthesized by simple hydrothermal methods and employed as supports for Ni catalysts in CO 2 methanation . Both of the nanostructured Ni/Al 2 O 3 catalysts displayed good activity. In comparison, the Ni/Al 2 O 3 -S catalyst showed higher CO 2 conversion than the Ni/Al 2 O 3 -P counterpart at the reaction temperature ranging from 250 to 400 °C. The physical and chemical properties of the catalysts were systematically characterized by N 2 sorption , X-ray diffraction (XRD), high resolution-transmission electron microscopy (HR-TEM), hydrogen temperature-programmed reduction (H 2 -TPR) and CO 2 temperature-programmed desorption (CO 2 -TPD) techniques. Higher specific surface area and stronger metal-support interactions were confirmed on the Ni/Al 2 O 3 -S catalyst, which may lead to smaller particle size of Ni nanoparticles . Moreover, the Ni/Al 2 O 3 -S catalyst possessed more abundant weak and medium basic sites, which would benefit the activation of CO 2 . The smaller Ni size and more suitable basic sites may rationalize the superior activity of the Ni/Al 2 O 3 -S catalyst. Besides, the Ni/Al 2 O 3 -S catalyst exhibited excellent stability at 325 °C for 40 h.
研究领域:
化学工程
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Wenhui Li,Yi Liu,Minchen Mu,Fanshu Ding,Zhongmin Liu,Xinwen Guo,Chunshan Song
Various organic acids were investigated for preparing the highly dispersed cobalt catalysts on zirconia support, Co/ZrO 2 , by an acid-assisted incipient wetness impregnation. The organic acid-assisted preparation results in highly dispersed Co/ZrO 2 catalysts which demonstrate superior catalytic activity with only 2 wt.% Co loading for CO 2 methanation. Among the acids, the carboxylic acids with bigger molecular weight, more carboxyl groups and hydroxyl groups are more effective. Furthermore, the amino acids can also change the charge property of ZrO 2 surface through controlling the solution pH and increase the metal dispersion through strong electrostatic adsorption. It is worth mentioning that, among the numerous organic acids, citric acid-assisted preparation gives Co/ZrO 2 catalyst with superior catalytic activity and increased the CO 2 conversion from 38% to 85% with highest turnover frequency. The linear relationship between metal dispersion and TOF with the molar ratio of acid to cobalt n CA/Co ranging from 0 to 2 demonstrates the importance of well dispersed metal particles in the enhanced activity. However, when the n CA/Co value exceeds 2 and the metal particle size further decreases, but no further enhancement is observed and the CO 2 conversion even slightly decreased at the n CA/Co value of 5. The organic acids-assisted strategy can lead to increased metal dispersion and higher TOF for Co/ZrO 2 catalysts; the appropriate metal dispersion corresponds to the suitable Co-ZrO 2 interaction with oxygen vacancy which leads to more catalytically active sites for CO 2 adsorption and catalytic hydrogenation. The organic acid-assisted strategy provides a new design approach for highly dispersed and active catalysts.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Tengfei Zhang,Peng Zheng,Jiajian Gao,Zhennan Han,Fangna Gu,Wenqing Xu,Fang Wang,Tingyu Zhu,Guangwen Xu,Ziyi Zhong,Fabing Su
Redispersing bimetallic active nanoparticles in a heterogeneous catalyst can significantly improve metal utilization and catalytic performance, but it is very challenging. In this work, we report a feasible method to redisperse large bimetallic NiRu particles (30–40 nm) on the CeO 2 support into small alloyed NiRu nanoparticles (3–5 nm) in an Ar gas atmosphere (NiRu/CeO 2 -Ar). During the high-temperature treatment, Ru metal in big bimetallic NiRu particles migrated to the surface of small alloyed nanoparticles because of the metal-phase separation, forming more Ni−Ru metal interfaces. As a result, NiRu/CeO 2 -Ar showed much better catalytic performance in CO 2 methanation than the pristine catalyst (NiRu/CeO 2 ) and the catalysts treated in air, H 2 , and reactant gases, respectively. Experimental and theoretical calculation results reveal that the newly generated Ni−Ru metal interfaces are conducive to the adsorption of CO 2 and further direct dissociation into CO*, thus enhancing the catalytic performance. This work provides a reliable strategy to redisperse bimetallic NiRu nanoparticles into small ones with more intermetallic interfaces.
研究领域:
化学工程
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
ADVANCES IN POLYMER TECHNOLOGY
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2017
·Vol. 37
·期 6
·2325-2335
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IF 1.291
Peng Zhou,Song Wang,ChuanLan Tao,Xingkui Guo,Luhan Hao,Qian Shao,Lei Liu,Ya-Ping Wang,Wei Chu,Bin Wang,Shi-Zhong Luo,Zhanhu Guo
Mesoporous alumina, as a porous, high specific surface area, high activity, and heat stable material, has been widely used as an industrial adsorbent, catalyst, and catalyst support. The modification of alumina with organic polymers has been widely investigated in recent years. In this study, we compared the dependence of the adsorption of a polyelectrolyte, poly(acrylic acid) (PAA) on γ-alumina particles on polymer size via Fourier transform infrared spectroscopy, thermogravimetry, nitrogen adsorption–desorption isotherm analysis, and atomic absorption spectrophotometry. We found that PAA with a hydrodynamic diameter greater than the alumina pore size would only adsorb on the outer surface of the oxides. For polymers with hydrodynamic diameters smaller than the alumina pore size, PAA infiltration resulted in a monolayer coverage of both the outer and inner surfaces of the oxide. Among the three PAA that could infiltrate the alumina pores, the one with the smallest molecular weight showed the highest adsorbed amount on alumina. The temperature, pH, concentration, and ionic strength of the PAA solutions were varied to illustrate the physicochemical differences of the prepared polymer/oxide composite materials. The high PAA-loaded composites were treated with a nickel ion solution, converted to Ni/alumina catalysts, and used in the methanation of carbon dioxide. The Ni/alumina catalysts were analyzed with X-ray diffraction and temperature-programmed reduction to illustrate the structural characteristics. The catalytic CO 2 methanation of the catalyst samples revealed that a solution pH value higher than p K a of PAA favored the formation of catalysts with high catalytic activity.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
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2025
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IF 13.1
Shaorong Deng,Chenji Zhu,Xiuzhong Fang,Xianglan Xu,Xiang Wang
A series of Ru-x%Li+/SiO2 catalysts (x = 0.05–0.2), modified with varying amounts of lithium cation (Li+), were prepared via coimpregnation and evaluated for CO2 methanation to explore Li+ modification on Ru/SiO2. Introducing trace Li+ markedly boosts reaction activity, with the optimal Ru-0.1%Li+/SiO2 exhibiting 38.4 and 12.3 times higher overall reaction rate and turnover frequency at 200 °C, respectively, compared to Ru/SiO2. Structural characterization confirmed that Li+ incorporation effectively suppresses RuO2 crystallization, thereby improving Ru dispersion from 9.1% to 31.5%, enhancing the active surface area from 33 to 115 m2 g–1, while simultaneously reducing Ru particle size from 18.4 to 3.2 nm. In situ spectroscopy and surface reaction experiments revealed that the CO* pathway occurs for CO2 methanation on both catalysts, which involves CO2 dissociation and subsequent CO* hydrogenation. The smaller Ru nanoparticles on Ru-0.1%Li+/SiO2 exhibit superior intrinsic activity for both steps compared to the larger nanoparticles on Ru/SiO2. The additional alkaline sites introduced by Li+ additives also promote CO2 dissociation. The exceptional activity of Ru-0.1%Li+/SiO2 for CO2 methanation is governed by the synergistic effect between the Ru particle size effect and Li+-induced basicity, with the former being predominant.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子