Catalysts
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2023
·Vol. 13
·期 5
·800
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IF 3.9
Zhong Xie,Jinpei Hei,Lei Cheng,Jing Li,Xiaojie Yin,Sugang Meng
CO2hydrogenation to methanol was conducted using a set of activated carbon-supported Cu/ZnO/Al2O3catalysts (CCZA) prepared by an incipient wetness impregnation approach. The effect of the Cu/Al ratio on the physicochemical properties of the catalysts, as well as their catalytic performance, were investigated. As Cu/Al ratio increased, the metallic Cu surface area displayed a reducing trend from 6.88 to 4.18 m2∙gcat−1, while the CO2adsorption capacity exhibited an increasing trend. Meanwhile, aluminum content will have an important effect on the catalysts’ reducibility and, thus, on their catalytic performance. The CCZA-2.7-de catalyst demonstrated the highest selectivity to methanol at 83.75% due to the excellent distribution and synergistic effect of copper and zinc. Although the CO2conversion of CCZA-2.2-de and CCZA-3.5-de exceeded 10%, the CH3OH selectivity was less than 60%, which may be attributed to the larger particle sizes of ZnO and poor interactions in Cu–Zn. The present study offers a novel approach to increase the number of active sites, optimize the activated carbon-aided Cu/ZnO/Al2O3catalyst’s composition, and finally elucidate the mechanism for CO2hydrogenation to methanol.Keywords:CO2hydrogenation;CuO/ZnO/Al2O3catalyst;methanol synthesis;carbon-supported catalyst;thermocatalysis
研究领域:
催化
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化学工程
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环境科学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Houde She,Suyue Cao,Jiufu Chen,Xiaoping Chen,Jingwei Huang,Lei Wang,Qizhao Wang
High indoor formaldehyde levels from residential decorations pose a pressing environmental concern, underscoring the urgency for effective catalytic degradation strategies. In this study, a La-doped ZnMn 2 O 4 catalyst with an oxygen-rich vacancy was successfully synthesized via a straightforward hydrothermal method. The experimental findings demonstrate that the L 0.5 ZMO catalyst, with a La doping amount of 0.5 mmol, exhibits a remarkable 100 % efficiency in degrading formaldehyde. Structural and spectroscopic analyses reveal that La doping in ZnMn 2 O 4 induces significant lattice expansion and an increased proportion of Mn 3 + species, both of which synergistically enhance the catalytic oxidation performance at room temperature. DFT results show that La doping concentrates the charge density near the Fermi energy level, significantly altering the charge distribution. This facilitates electron transfer, leading to enhanced photocatalytic performance. Furthermore, the introduction of oxygen vacancies generates abundant active sites, substantially improving the formaldehyde decomposition efficiency. This study highlights the critical role of La incorporation in modulating oxygen vacancies and surface properties of ZnMn 2 O 4 , yielding a cost-effective catalyst for efficient indoor formaldehyde abatement under ambient conditions.
研究领域:
环境科学
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材料化学
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催化
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纳米技术
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室内空气质量
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产品关联
DOI
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2023
·Vol. 49
·期 9
·3933-3950
·
IF 3.3
Li Xiaojun,Xia Yudong,Xu Yangzhou,Li Haitao,Huang Jiangchao,Yao Jie,Zhao Heng,Gao Xinhua,Yu Jinghao,Guo Lisheng,Li Jie
Thermocatalytic conversion of redundant CO 2 to useful methanol is an attractive route to address both energy and environmental crises simultaneously. However, existing copper/oxide catalysts widely used in these thermocatalytic processes still suffer from low methanol yield under mild reaction conditions. In this work, we design inverse oxide/Cu catalysts to achieve superior thermal catalytic performance for CO 2 hydrogenation. The optimized ZnO/Cu-1.0 catalyst exhibits maximum CH 3 OH selectivity of 83.4% and space–time yield (STY) of \(170.9\;{\text{g}}_{{{\text{CH}}_{3} {\text{OH}}}} \;{\text{kg}}_{{{\text{cat}}}}^{ - 1} \;{\text{h}}^{ - 1}\) in CO 2 hydrogenation at 210 °C, nearly twofold higher STY than the previous optimal inverse ZnO/Cu catalysts ( \(89.6\;{\text{g}}_{{{\text{CH}}_{3} {\text{OH}}}} \;{\text{kg}}_{{{\text{cat}}}}^{ - 1} \;{\text{h}}^{ - 1}\) at 250 °C). Importantly, ZnO/Cu-1.0 catalyst displayed not only a satisfactory catalytic stability but also a superior CH 3 OH STY with a time-on-stream of 24 h. Such inverse configuration of catalysts will pave the way for new strategies to design high-performance thermocatalytic catalysts and promote their commercialization. Graphical abstract Typical inverse ZnO/Cu-1.0 catalysts have been demonstrated and achieved to significantly facilitate the activation of inert CO 2 molecules to produce methanol, due to its special physicochemical properties and strong ZnO–Cu interaction
研究领域:
催化
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化学工程
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材料科学
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环境科学
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能量转换
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DOI
高影响因子
Advanced Healthcare Materials
·
2024
·
IF 10
Jiaxin Dong,Guanxiong Liu,Yuri V. Petrov,Yujie Feng,Dechang Jia,Vladimir E Baulin,Aslan Yu Tsivadze,Yu Zhou,Baoqiang Li
Iron phosphide/carbon (FeP/C) serving as electrocatalysts exhibit excellent activity in oxygen reduction reaction (ORR) process. H 2 O 2 catalyzed by peroxidase (POD) is similar to the formation of new electron transfer channels and the optimization of adsorption of oxygen-containing intermediates or desorption of products in ORR process. However, it is still a challenge to discover FeP/C with enhanced POD-like catalytic activity in the electrocatalytic database for biocatalysis. The discovery of FeP/carbon dots (FeP/CDs) nanozymes driven by electrocatalytic activity for enhanced POD-like ability is demonstrated. FeP/CDs derived from CDs-Fe 3+ chelates show enhanced POD-like catalytic and antibacterial activity. FeP/CDs exhibit enhanced POD-like activities with a specific activity of 31.1 U mg −1 that is double higher than that of FeP. The antibacterial ability of FeP/CDs nanozymes with enhanced POD-like activity is 98.1%. The antibacterial rate of FeP/CDs nanozymes (250 µg mL −1 ) increased by 5%, 15%, and 36% compared with FeP, Fe 2 O 3 /CDs, and Cu 3 P/CDs nanozymes, respectively. FeP/CDs nanozymes will attract more efforts to discover or screen transition metal phosphide/C nanozymes with enhanced POD-like catalytic activity for biocatalysis in the electrocatalytic database.
研究领域:
材料科学
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纳米技术
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生物化学
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催化
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生物医学工程
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
He Tiwei,Tang Hongchao,Wu Jie,Wang Jiaxuan,Zhang Mengling,Lu Cheng,Huang Hui,Zhong Jun,Cheng Tao,Liu Yang,Kang Zhenhui
Carbon-based metal-free catalysts are promising green catalysts for photocatalysis and electrocatalysis due to their low cost and environmental friendliness. A key challenge in utilizing these catalysts is identifying their active sites, given their poor crystallinity and complex structures. Here we demonstrate the key structure of the double-bonded conjugated carbon group as a metal-free active site, enabling efficient O 2 photoreduction to H 2 O 2 through a cascaded water oxidation − O 2 reduction process. Using ethylenediaminetetraacetic acid as a precursor, we synthesized various carbon-based photocatalysts and analyzed their structural evolution. Under the polymerization conditions of 260 °C to 400 °C, an N -ethyl- 2 -piperazinone-like structure was formed on the surface of the catalyst, resulting in high photocatalytic H 2 O 2 photoproduction (2884.7 μmol g −1 h −1 ) under visible light. A series of control experiments and theoretical calculations further confirm that the double-bond conjugated carbonyl structure is the key and universal feature of the active site of metal-free photocatalysts.
研究领域:
材料科学
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催化
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光化学
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产品关联
DOI
PubMed
高影响因子
Catalysts
·
2019
·Vol. 9
·期 5
·399
·
IF 3.444
Boyu Du,Bingyang Liu,Yingying Yang,Xing Wang,Jinghui Zhou
Obtaining renewable fuels and chemicals from lignin is an important challenge in the use of biomass to achieve sustainability and energy goals. At present, acid-based catalysts for lignin depolymerization are considered to be a potential but challenging way to produce low-molecular-mass aromatic chemicals. The main concerns with the use of Lewis acids and zeolite catalysts are the corrosive nature of the acids, the possible formation of unwanted byproducts, and the possible formation of harsh reaction conditions. We achieved high-yield conversion using phosphotungstic acid (PTA) polyoxometalate catalysts in ethanol/water under different reaction conditions with little formation of bio-char. The monomeric products were mainly composed of various types of aromatic compounds. Our method does not require the use of precious metals and harsh reaction conditions—it only requires relatively mild reaction conditions and homogeneous catalysis—thereby greatly reducing operating costs and increasing the yields. Therefore, this PTA catalyst, which has excellent performance in bulrush lignin catalysis, would be a good alternative to the traditional catalysts used in lignin depolymerization and have wide application in biomass use.Keywords:lignin;catalytic depolymerization;phosphotungstic acid catalyst;β-O-4
研究领域:
可再生能源
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催化
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生物质转化
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化学工程
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产品关联
DOI
高影响因子
Science Advances
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2024
·Vol. 10
·期 47
·
IF 11.7
Rongrong Pan,Qi Wang,Yan Zhao,Zhendong Feng,Yanjun Xu,Zhuan Wang,Yapeng Li,Xiuming Zhang,Haoqing Zhang,Jia Liu,Xiang-Kui Gu,Jiangwei Zhang,Yuxiang Weng,Jiatao Zhang
Sluggish surface reaction is a critical factor that strongly governs the efficiency of photocatalytic solar fuel production, particularly in CO2-to-ethanol photoconversion. Here, inspired by the principles underlying enzyme catalytic proficiency and specificity, we report a biomimetic photocatalyst that affords superior CO2-to-ethanol photoreduction efficiency (5.5 millimoles gram−1 hour−1 in average with 98.2% selectivity) distinctly surpassing the state of the art. The key is to create a class of catalytic pocket, which contains spatially organized NH2…Cu-Se(-Zn) multiple functionalities at close range, over ZnSe colloidal quantum wells. Such structure offers a platform to mimic the concerted cooperation between the active site and surrounding secondary/outer coordination spheres in enzyme catalysis. This is manifested by the chemical adsorption and activation of CO2 via a bent geometry, favorable stabilization toward a variety of important intermediates, promotion of multielectron/proton transfer processes, etc. These results highlight the potential of incorporating enzyme-like features into the design of photocatalysts to overcome the challenges in CO2 reduction.
研究领域:
化学
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材料科学
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催化
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产品关联
DOI
PubMed
高影响因子
CARBON
·
2024
·
IF 10.5
Hao Wen,Fubin Ma,Haoyang Li,Yi Yue,Jiacheng Luo,Ruiyang Qu,Hepeng Zhang,Yueling Cao
Fabrication of metal/porous carbon catalysts with high catalytic activity and stability is highly desirable but challenging because the metal nanoparticles in these catalysts cannot have both high exposure and strong interaction with carbon support. Here, for the first time, a facile CO 2 -assisted one-pot pyrolysis (CAOP) strategy was developed to in situ liberate the inaccessible Ru sites without obviously affecting the size of Ru nanoparticles . The Ru@CN-700-80 prepared with the assistance of CO 2 exhibits a remarkable improvement in catalytic activity for levulinic acid hydrogenation compared with that without CO 2 during pyrolysis, giving a TOF of 28449 h −1 under mild conditions, which is superior to the reported Ru-based catalysts. Additionally, the Ru@CN-700-80 also demonstrates an excellent stability without activity loss after 10 cycles. We anticipate that this CAOP strategy addresses a crucial issue that currently plagues the design of metal/porous carbon catalyst with high catalytic performance applied in energy and environmental fields.
研究领域:
催化
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化学工程
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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
APPLIED CATALYSIS A-GENERAL
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2020
·
IF 5.006
Xiao Chen,Jianyu Li,Yue Wang,Ying Zhou,Qiulian Zhu,Hanfeng Lu
Metal-based monolithic catalysts have excellent electrical and thermal conductivity, impact resistance, ductility, and mechanical properties. Thus, they have a broader application prospect than ceramic-based monolithic catalysts. In this work, high-dispersion Pd nanoparticle dispersion liquid was synthesized by using the solvothermal method. Moreover, nickel-foam-supported Pd/NiO (Pd/NiO/Ni foam) monolithic catalyst with good catalytic combustion performance was prepared successfully by simply spraying the dispersion liquid on the surface of Ni foam, which was oxidized at high temperature to grow NiO film. A novel electric heating catalytic combustion reactor with fast response and safety was constructed by nesting Pd/NiO/Ni foam with an insulated heating rod. Notably, even at the high space velocity of 50,000 h −1 , the constructed reactor can completely degrade 2500 ppm of toluene at 230 ℃ and exhibits good catalytic activity for hydrocarbons and oxygen-containing and heteroatom-containing organic compounds.
研究领域:
催化
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环境工程
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
OPTICAL MATERIALS
·
2023
·
IF 3.9
Ning Zhang,Rong Wu,Yu Zhang,Jianyong Yue,Haitong Jing,Shunhang Wei,Fangping Ouyang
The photocatalytic activity of Bi 4 Ti 3 O 12 is limited by the lack of active sites and rapid carrier recombination. In this work, the problems mentioned above are effectively solved by using a dual functional CuS load on the surface of Bi 4 Ti 3 O 12 . The CuS can be used as electron trapping sites to play a role as a cocatalyst, and form p-n junction with the Bi 4 Ti 3 O 12 under irradiation through the properties of p-type semiconductor. The dual functionality of CuS effectively promotes carrier separation and enhances the photocatalytic degradation activity. The photocatalytic rate of Bi 4 Ti 3 O 12 with optimal loading amount of CuS is ∼1.8 and ∼2.7 times as high as that of the Bi 4 Ti 3 O 12 and the CuS, respectively. The photocatalytic mechanism of the Bi 4 Ti 3 O 12 –CuS system is investigated in detail.
研究领域:
材料科学
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环境科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
DIAMOND AND RELATED MATERIALS
·
2023
·
IF 4.1
Fengling Wang,Sen Jin,Yaqiong Du,Qixun Xia,Libo Wang,Aiguo Zhou
Mo 2 C T x is a novel co-catalyst to enhance the photocatalytic performance of CdS for H 2 production. The surface of Mo 2 C T x is usually terminated by fluorine anion because it is generally made by the etching of fluoride-containing solution. Here we report, a novel method to prepare highly pure MXene with Br termination by the etching of pure HBr at 220 °C for 3 d, or the HBr solution mixed with LiBr, NaBr, KBr or NH 4 Br at 180 °C for 24 h. The pure HBr etching needs higher temperature and longer time to make pure Mo 2 C T x , however, which result lager interlayer space and more active sites. All the Mo 2 C T x samples show high co-catalytic performance to enhance the photocatalytic performance of CdS for H 2 production. The H 2 production rate of CdS combined with HBr etched sample was 17,566 μmol g −1 h −1 , similar with the sampled combined with traditionally HF etched sample. This is the first report to prepare MXene by etching of Br containing solution. The Mo 2 C T x made by this method is terminated by Br/O without F, and show excellent co-catalytic properties.
研究领域:
材料科学
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化学
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催化
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xinyi Li,Jingjing Liu,Qinghai Cai,Ziwang Kan,Song Liu,Jingxiang Zhao
Modulating the microenvironment of single-metal active sites holds excellent promises for developing highly efficiently oxygen electrocatalysts. Herein, by combining theoretical predictions and experiments, we reported a general strategy to engineer the electronic properties of iron-nitrogen-carbon (FeN 4 /C) catalysts via the incorporation of the boron (B) atom for achieving improved catalytic activity in oxygen electrocatalysis. Our theoretical results revealed that B modulation effectively tunes the d-band center of the iron (Fe) active site to optimize its adsorption strength with oxygenated species, greatly enhancing oxygen reduction reaction (ORR) and oxygen evolution reactions (OER) activity. Our experimental measurements then confirmed the above theoretical predictions: the as-synthesized B-doped FeN 4 /C (Fe-N 4 -B) material can perform as an eligible bifunctional catalyst for ORR and OER in alkaline media, and its catalytic activity even outperforms the commercial noble metal benchmarks. The present findings provide a promising strategy to further design the advanced catalysts for a wide range of electrochemical applications.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）