JOURNAL OF CATALYSIS
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2025
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IF 6.5
Mengjie Cao,Shuangde Li,Shikun Wang,Weichen Xu,Xin Zhou,Guangxin Ma,Yunfa Chen
Developing an efficient and environmentally friendly catalyst is important for the production of pure H 2 and carbon nanomaterials. Catalytic cracking of methane offers the possibility of producing these high-value products. For this reason, stabilizing the surface active sites of activated methane by modulating the interaction between metal and support has attracted much attention in the development of hydrotalcite-derived NiAl catalysts. Hence, the influence of Zn content and cracking temperature on the structure and performance of hydrotalcite-derived NiZnAl methane cracking catalysts were investigated. It is shown that alloying Zn with Ni reduces the electron density near Ni atoms, promotes the reduction of mixed metal oxides, producing strong interactions between Ni and support, thus improving the stability of the catalyst during methane decomposition. Thus, this strong interaction between Ni and support stabilized the Ni particle size and inhibited the sintering of Ni during the reaction. The Ni 2.7 Zn 0.3 Al can maintain a H 2 yield of more than 60 % over a 600 min reaction time at 600 °C. TEM analysis showed that the strong metal support interaction changed the morphology of the deposited carbon, maintained the balance between carbon diffusion and CH 4 dissociation, provided more growth sites for carbon nanotubes, and also prevented the rapid deactivation of the catalysts because of carbon encapsulation. This article may provide guidance for the design of Ni-based methane cracking catalysts with excellent stability.
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
ACS Catalysis
·
2019
·
IF 12.221
Jian Li,Yaping Lin,Xiulian Pan,Dengyun Miao,Ding Ding,Yi Cui,Jinhu Dong,Xinhe Bao
Strong metal–support interaction (SMSI) has been widely recognized for platinum-group metals on reducible oxide supports. Herein we report that the catalytic activity of Ni catalyst in CO2 methanation is significantly suppressed over conventional anatase (a-TiO2) support due to the SMSI-induced formation of a titania overlayer around the Ni nanoparticles. Furthermore, CO is the only product . In contrast, the NH3-treatment and H2-treatment of the a-TiO2 support enhance remarkably the activity of Ni, i.e., CO2 conversion increases by 1 order of magnitude and CO2 is hydrogenated almost exclusively to CH4. X-ray photoelectron spectroscopy (XPS), H2 and CO chemisorption, and low temperature electron paramagnetic resonance (EPR) reveal that the enhanced CO2 methanation activity may be related with the Ti3+ species in the bulk that are generated by reduction treatment, which likely have altered the SMSI between Ni and a-TiO2 support. This simple reduction treatment approach may be applicable to modulate the SMSI of other reducible oxide-supported metal catalysts.
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
Catalysts
·
2022
·Vol. 12
·期 10
·1286
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IF 4.501
Ravi Balaga,Kishore Ramineni,Xiaoqiang Zhang,Peifang Yan,Mahender Reddy Marri,Vijayanand Perupogu,Zongchao Conrad Zhang
Conversion of biomass-derived furfural (FFA) platform molecule to value-added tetrahydrofurfuryl alcohol (THFA) molecule is a sustainable route using an efficient non-noble metallic catalyst in water solvent. In this work, Ni in various loadings on mesoporous titanium dioxide (m-TiO2) was synthesized in one pot by Evaporation-Induced Self-Assembly (EISA). The synthesised catalysts were evaluated for the hydrogenation of furfural to tetrahydrofurfuryl alcohol. The catalysts were characterised using a combination of spectroscopic techniques such as XRD, H2-TPR, H2-TPD, XPS, SEM-EDX, TEM, and HR-TEM. The characterization results show that the Ni/m-TiO2materials exhibit enhanced electron-rich active sites, facilitated hydrogen spillover, uniform dispersion of small Ni particles (~5 nm), and strong metal support interaction between Ni and TiO2. Among the various Ni dopings, 7.5 wt.% Ni/m-TiO2catalyst exhibited the best performance and achieved 99.9% FFA conversion and 93.2% THFA selectivity in water solvent at 100 °C and under 2 MPa H2. Additionally, detailed kinetic studies, process parameters, the stability and reusability of the catalyst were also studied. The results demonstrated that the 7.5 wt.% Ni/m-TiO2catalyst is highly active and stable.Keywords:biomass;furfural hydrogenation;electron-rich Ni;SMSI;spillover
研究领域:
催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
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2016
·Vol. 6
·期 74
·70424-70432
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IF 3.289
Ran Ji,Shangru Zhai,Wei Zheng,Zuoyi Xiao,Qingda An,Feng Zhang
Towards the aerobic oxidation of alcohols, palladium nanoparticle immobilized mesoporous catalysts have been extensively investigated; however, the preparation of efficient catalytic materials without using complexing moieties remains a challenge. Herein, a simple yet effective concept that directly utilizes inorganic ZrSBA-15, a mild acidic framework, as a supporting matrix for Pd NPs was applied. The catalysts were fully characterized using X-ray diffraction, N2 adsorption–desorption isotherms, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy. It was demonstrated that, on the basis of these characterization results, active Pd NPs had been successfully loaded onto the porous framework of ordered ZrSBA-15. More significantly, the method of preparation was also attributed to the catalytic properties of the resultant sample, in which the interactions between Pd species and acidic framework were improved, leading to a uniform dispersion and enhanced stabilization of Pd particles. Meanwhile, Pd/ZrSBA-15 catalysts exhibited expected activity in the aerobic oxidation of benzyl alcohol with at least 95% conversion and 99% selectivity for benzaldehyde. Moreover, the oxidation reaction could be performed smoothly under solvent- and base-free conditions, and the catalyst was recycled several times with negligible loss in selectivity and conversion.
研究领域:
化学
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2018
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IF 3.525
Shengyang Wang,Bin Zeng,Can Li
Plasmonic photocatalysis with tunable light absorption has aroused significant attention in solar-to-chemical energy conversion. However, the energy conversion efficiency of plasmonic photocatalysts is impeded by ineffective charge separation and the lack of highly active sites for redox reactions. In this work, the Au nanoparticle size and Au-TiO 2 interaction of the Au/TiO 2 plasmonic photocatalyst were adjusted simultaneously using a post-calcination treatment. The visible-light-induced water oxidation activity exhibited a volcano-like relationship with the calcination temperature; the treated photocatalyst at 600 °C manifested the highest activity. Characterization with UV-visible spectra, XRD, SEM, and XPS revealed that the effect of the Au nanoparticle size and Au-TiO 2 interaction were both responsible for the increase in plasmon-induced water oxidation activity.
研究领域:
材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2018
·Vol. 42
·期 22
·18381-18387
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IF 3.201
Hang Cheong Chan,Ting Chen,Lifang Xie,Yijin Shu,Qingsheng Gao
As promising catalyst supports, hydrogenated metal-oxides can afford engineered surface architectures and electronic configurations to promote catalytic turnover on loading metals. Herein, hydrogenated TiO2 (H-TiO2) fabricated via NaBH4 reduction is successfully introduced to boost the catalytic oxidation of formaldehyde (HCHO), which is one of the most common and harmful indoor volatile organic compounds. Distinct from the parent TiO2, H-TiO2 features enriched surface hydroxyls and enhanced metal–support interactions upon loading Ir, which are responsible for remarkable promotion in HCHO oxidation. In particular, the abundant hydroxyls on H-TiO2 promote the generation of HCOO−, which is believed to be the rate-determining step in HCHO oxidation. This discovery is anticipated to pave the way for exploring high-performance metal catalysts on oxide supports via surface and interfacial engineering.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Zequn Zhang,Yuan Shu,Qian Liu,Shuxian Bi,Pengfei Zhang
Colloidal nanoparticles with uniform particle size distribution, tailored exposed facets, and controllable compositions appealed to broad interests in heterogeneous catalysis. Nevertheless, due to the strong attachment of capping agents to the nanoparticles, cleaning the nanoparticle surface without changing the size of nanoparticles remains a significant challenge. Herein, based on the double confinement of the strong metal-support interaction (SMSI) effect and carbon encapsulation, the well-stabilized Ni-ZnO-S3 catalyst was successfully synthesized. The size of Ni nanoparticles after calcination in the sequence of H 2 -N 2 mixture, air, and H 2 -N 2 mixture remained below 5 nm. Due to no significant size change in Ni nanoparticles, the prepared Ni-ZnO-S3 catalyst served well as model catalysts in the RWGS reaction, where the CO 2 conversion and CO yield increased proportionally to the Ni loading weight. According to the result of in-situ FTIR, an associative mechanism of RWGS reaction over Ni-ZnO-S3 was also identified. Therefore, this dual protect strategy provides a potential solution for building highly anti-sintering catalysts based on the colloidal synthesis route.
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
Catalysis Science & Technology
·
2023
·Vol. 13
·期 15
·4489-4497
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IF 5
Kewu Yang,Ke Wang,Xianfeng Shen,Fanxing Zhang,Bei Huang,Keping Yan,Yao Shi,Yi He,Pengfei Xie
The exposed facets of ceria crystals have a profound effect on the reactivity of ceria-supported catalysts owing to the intricate metal–support interactions. In this work, ceria nanorods, nanocubes, and polyhedra, with corresponding exposed (110)/(100), (100), and (111) terminations, were hydrothermally synthesized to support Pd species, with the aim of investigating the in-depth impacts of ceria crystal facets for methane combustion over ceria-supported palladium catalysts. The nanorod sample delivered the highest methane conversion (T50 = 277 °C, GHSV = 200 000 mL h−1 gcat−1) and greater reaction rate (9.59 × 10−4 molCH4 h−1 gcat−1), 1.23 times that of nanocubes and 3.14 times that of polyhedra. Further characterizations revealed that on the (110)/(100) surface planes, PdOx exhibited stronger interactions with CeO2. This led to enhanced formation of Pd4+ and higher reducibility of PdOx species, thus promoting methane activation. This work would supply experimental insights into the relationship between exposed facets and reactivity, as well as guidance for rational catalyst design.
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
MICROCHEMICAL JOURNAL
·
2024
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IF 4.9
Ziping Li,Qijie Mo,Guiyan Li,Xian Wang,Junjie Shao,Yao Zhang,Jian Chen,Zhijun Chen,Jingwen Tan,Zhenji Wang,Yijin Shu,Qingsheng Gao
Supported metal nanomaterials have great potential in catalytic sensing, but the poor selectivity and easy aggregation of noble metals limit their development in non-enzyme sensing applications. Herein, this research focuses on the metal-support interactions of Pd supported on PCN-222, exploring the role of abundant porphyrin groups on the PCN-222 surface and the tuning of Pd composition to enhance electron configuration. Through the anchoring of PCN-222 surface to Pd species and utilizing the confining effect of open channels, the Pd@PCN-222 nanostructures with uniform particle size of Pd were successfully obtained. Strong electron interaction can enhance the catalytic activity of Pd@PCN-222 towards reaction, while increasing the Pd loading can improves the sensitivity of the sensors in the high concentration of H 2 O 2 . Combining the above two points, 0.29 %-Pd@PCN-222 exhibits a low detection limit of 0.27 μM and a wide linear range of 1–1000 μM in H 2 O 2 sensing via using a colorimetric method. Experimental and theoretical results show that Pd@PCN-222 exhibit strong p - d orbital coupling and adsorption, and rapid catalytic kinetics towards H 2 O 2 , enhancing the overall catalytic process. At the same time, DFT calculations are used to simulate the material surface and sensing process, which also enrich the research content of MOF materials in sensing. From the structure-performance relationships to the directly analyze the H 2 O 2 in real samples, this work is expected to provide some guidance for the development of efficient sensing systems.
研究领域:
材料科学
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催化化学
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
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IF 8.035
Haiping Yang,Shuai Yan,Dingding Yao,Hao Luo,Kuo Zeng,Jun Li,Dian Zhong,Haoyu Xiao,Hanping Chen
A novel photo-thermal catalytic pyrolysis of LDPE was conducted with a solar simulator for effective and energy-conserving production. Four photothermal catalysts, including TiO 2 , NiTi(Ni/TiO 2 ), NiAl(Ni/Al 2 O 3 ) and NiTiAl(Ni/TiO 2 /Al 2 O 3 ), were prepared to study the performance on gas and carbonaceous production at variant temperatures (500 °C, 600 °C and 700 °C). NiTiAl reached carbon nanotubes(CNTs) yield of 280 mg/g plastics with simultaneous hydrogen yield of 54 mmol/g even at 700 °C. For the better understanding of light-induced carbon deposition and hydrogen evolution, pyrolysis in pure thermal mode was also carried out over NiTiAl for comparison, where H 2 production of 28 mmol/g and little carbon product was found. It turns out that the introduction of irradiation together with support component deliberately mediated the metal-support interaction in NiTiAl by certain photoelectrons transfer, which was favorable for CNTs growth and hydrogen evolution. It is expected to provide a design strategy of catalysts in solar pyrolysis of carbonaceous feedstock.
研究领域:
环境科学
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材料科学
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能源科学
✓ 已验证
DOI
高影响因子
ACS Catalysis
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2022
·
IF 13.7
Xiao-Chen Sun,Kun Yuan,Wang-De Hua,Zi-Rui Gao,Qian Zhang,Chen-Yue Yuan,Hai-Chao Liu,Ya-Wen Zhang
The metal–support interface plays a crucial role in heterogeneous catalysis. The modulation of the metal–support interaction (MSI) affords the possibility of promoting the catalytic efficiency per active site. Here, we report a strategy to modulate the interfacial interaction and then optimize the interfacial activity of Co/CeO2 catalysts for the water–gas shift reaction (WGSR) by a facile NH3 treatment process for the CeO2 support. The sample of Co/800N-CeO2 treated at 800 °C exhibited the highest reaction rate of 260 μmolCO/(gCo s), which was 23.8 times higher than the rate of the untreated Co/CeO2 sample. A combination of ex situ and in situ characterizations suggested that addition of the NH3 treatment process did not only weaken the metal–support interaction between the Co species and CeO2 support to strengthen CO adsorption and CO activation ability but also induced oxygen vacancy generation under reaction conditions to accelerate H2O activation. Both worked together in promoting the catalytic efficiency for the WGSR via the carboxyl pathway at a low temperature. It was worth mentioning that the N species of the CeO2 support introduced by the NH3 treatment was removed after changing the catalyst structure under reaction conditions. The interfacial structure was robust in a 60 h test at 400 °C due to the coexistence mechanism of carboxyl and formate pathways avoiding the poisoning effect of formate species on the active sites. The construction of active interfaces could be extended to Fe/CeO2 and Ni/CeO2 catalysts and could bring great promise in the design of the interfacial structure of supported catalysts in wide applications including chemical transformation reactions and industrial catalysis.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Zhongrui Li,Lei Guo,Wenchen Ren,Junjie Han,Santosh Kumar Verma,Shihang Xu,Lin Liu,Tong Zhang,Yunhua Xu
The design of efficient ammonia cracking catalysts is the key to developing ammonia as a hydrogen storage carrier. This paper investigated the role of Co–Al hydrotalcite carriers in ruthenium-based catalysts. Ru/Co–Al catalysts were prepared by mechanical milling, impregnation, and co-precipitation, and the catalytic activity and physicochemical properties of the catalysts were investigated, respectively. The catalysts prepared by the co-precipitation method exhibit the maximum specific surface area and metal dispersion due to the layered structure of LDH and the homogeneity of the co-precipitation method. In this study, it is concluded that the substitution of Ru during the co-precipitation preparation builds up strong metal-carrier interactions and generates a large number of oxygen vacancies. The catalyst prepared by the co-precipitation method exhibited a high H 2 generation rate (19.5 mmol·gcat −1 ·min −1 ) at GHSV = 30,000 ml·gcat −1 ·h −1 and 450 °C, and the performance remained stable after 50 h of reaction. This work provides a new idea for designing efficient Ru-based catalysts.
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
危险品化学品经营许可证（带存储）