Nano Research
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2019
·Vol. 12
·期 4
·869-875
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IF 8.515
Long Yan,Li Jian,Wu Lanlan,Wang Qishun,Liu Yu,Wang Xiao,Song Shuyan,Zhang Hongjie
The Pt-Ni nanoframe catalysts have attracted great interest owing to their unique electronic structure and excellent catalytic performance. However, the stability of the tenuous edges of nanoframe-structures is dissatisfactory and their universal applications in catalytic market beyond electrocatalytic reactions are yet to be tapped and explored. Herein, we developed a new core@shell structured Pt-Ni nanoframe@CeO 2 (Pt-Ni NF@CeO 2 ) composite via etching the Ni from inhomogeneous Pt-Ni rhombic dodecahedra (Pt-Ni RD) by cerium(III) acetate hydrate (Ce(OAc) 3 ). In this path, Pt-Ni RD was used as self-sacrificial template, while the Ce(OAc) 3 serves as the provider of the Ce 3+ source and OH − for the formation of CeO 2 shell, etchant of Pt-Ni RD, and the surface modification agent. By this way, the etching of Pt-Ni RD and the formation of the CeO 2 shell are simultaneously proceeded to form the final Pt-Ni NF@CeO 2 in one step. The obtained Pt-Ni NF@CeO 2 exhibits strong interfacial charge transfer interaction between Pt-Ni NF core and CeO 2 shell even without reduction treatment, leading to enhanced catalytic activity in the hydrogenation of phenylacetylene. After introduction of trace silver, the Pt-Ni-Ag 4.9 NF@CeO 2 achieves remarkable catalytic performance for the selective conversion of phenylacetylene to styrene: high conversion (100%), styrene selectivity (86.5%), and good stability. It reveals that encapsulation noble metal nanoframes into metal oxide to form core@shell structured hybrids will indeed enhance their stability and catalytic properties. Particularly, this work expends the application of noble metal nanoframes materials to hydrogenation reactions.
研究领域:
催化材料
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纳米技术
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化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Shuaiqi Zhao,Jiajin Lin,Wenqiang Gong,Aihua Xu,Xiaoxia Li,Yongcai Qiu
Pt-based catalysts are one of the most extensively used heterogeneous catalysts for the degradation of pollutants, and regulating electron-metal-support interaction (EMSI) is an efficient strategy to enhance the performance of Pt-based catalysts. Herein, we introduced a quenching technique for regulating the EMSI of Pt-CuO/CeO 2 catalysts to significantly boost its CO catalytic activity. The EMSI optimized by quenching was determined to promote the electron redistribution between Pt and CuO/CeO 2 via Cu–O-Pt structure, thus forming more electron-rich Pt species and enhancing the surface oxygen species activity. From comprehensive characterization investigations, we confirmed that the superior activity arouse from the moderate Pt 0 /Pt 2+ ratio, in which CO molecules were preferentially adsorbed on the electron-rich Pt sites and reacted with active oxygen species from PtO x or CuO/CeO 2 , accelerating the whole CO catalytic process. Our finding provided a new inspiration to control EMSI of Pt-based catalysts and widened the application of quenching chemistry in heterogeneous catalysis.
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APPLIED CATALYSIS A-GENERAL
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2023
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IF 5.5
Lu Ji,Fang Li,Conghui Che,Wei Xue,Qiusheng Yang,Xiaoshu Ding,Dongsheng Zhang,Xinqiang Zhao,Yanji Wang
In the reaction of dimethyl carbonate (DMC) and 2,4-diaminotoluene (TDA), Au/CeO 2 exhibits higher selectivity than CeO 2 for dimethyl toluene-2,4-dicarbamate (TDC). However, its catalytic activity drops after H 2 reduction (denoted as Au/CeO 2 -R). The characterization results illustrate that Au exists as a single atom with the primary species as Au δ+ in Au/CeO 2 , forming Ce x Au 1−x O 2 structure similar to solid solution. Whereas for Au/CeO 2 -R catalyst, Au mainly exists as Au 0 , forming the Au-O-Ce structure on CeO 2 surface. Significantly, the strong interaction between Au and CeO 2 increases Ce 3+ and oxygen vacancies content, as well as modulates their acidic property. However, the catalytic activity of Au/CeO 2 -R is found to be lower than Au/CeO 2 as the species formed by DMC dissociation on its surface are not easily desorbed. Other transition metals supported on CeO 2 are also prepared, wherein Pt/CeO 2 and Pd/CeO 2 exhibit good TDC selectivity. In the end, the electronegativity and catalytic activity of metals are correlated.
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ELECTROCHIMICA ACTA
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2023
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IF 6.6
Zixiang Su,Hehe Wei,Longtao Zhang,Hui Li,Ping Liu,Zhenshan Hou,Xueqing Gong
The electrocatalytic oxygen reduction reaction (ORR) is the key bottleneck of fuel cells and rechargeable metal-air batteries , and recently, metal nitrogen complex carbon (M N C) demonstrates great potential in these fields. However, the complex and easily degraded M N C structure often results in inferior activity and poor durability in electrolysis. Herein, we fabricate a catalyst of h-CeO 2 @CoNC through the extended Stöber method and subsequent pyrolysis , involving the hollow CeO 2 as the core and Co N C as the shell. The h-CeO 2 @CoNC catalyst exhibits notable ORR catalytic performances in 0.1 M KOH with a half-wave potential of 0.82 V and excellent durability, attributed to the synergistic interaction between CeO 2 and Co N C matrix. Specifically, the inner layer of CeO 2 is principally responsible for enhancing the chemical stability and the outer one of Co N C matrix is beneficial to boosting the ORR catalytic activity. This work provides an efficient preparation approach and further insight of rational design of the unique M N C catalysts for energy storage.
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APPLIED ENERGY
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2023
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IF 11.2
Xiangyu Yan,Buchu Lu,Hao Dong,Qibin Liu
Combining solar light and heat in dry reforming of methane (DRM) is a promising technology for reducing CO 2 to a valuable syngas and increasing the utilization of solar light in the solar-to-fuel process. The reaction temperature is still high and the mechanism remains unclear in DRM. Clarifying the synergistic mechanism of solar light and heat is pivotal for industrial applications. To this end, a nanoscale Ni/CeO 2 catalyst is prepared, and the synergistic effect of solar light and heat in DRM is experimentally investigated. The experimental results show that photo-thermochemistry leads to a 39.74% increase in relative conversion rate of CH 4 compared to thermochemistry, while the reaction temperature is reduced by 45 °C. The syngas production rate and the selectivity of DRM are improved by solar light. The in-situ infrared study indicates that solar light enhances the dissociation process of CH 4 and the production of HCOO ⁎ on the surface of the Ni/CeO 2 catalyst. The light response in the catalyst and microscopic enhancement of intermediate products are responsible for the increased DRM performance under photo-thermochemical conditions. These findings contribute to the understanding of the synergistic effects of solar light and heat, and guide the conversion of CO 2 into fuel with the aid of solar energy.
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MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Congcong Yao,Junchao Qian,Feng Chen,Yaping Wang,Jinyu Lin,Jianping Chen,Jianqiang Wei,Zeling Yang
Water quality monitoring requires new water sensors with highly sensitive and low-power consumption to detect the increasingly widespread contamination of antibiotics. Quantum dots (QDs), typically solid solution quantum dots (SSQDs), are emerging as promising sensing materials candidates owing to their unique structure with extremely small size and extraordinary electronic properties. In this work, Zn-doped CeO 2 solid solution quantum dots with 2–6 nm grain size were embedded into biocarbon sheets and constructed as modified sensing electrode to detect trace ciprofloxacin (CIP). Biocarbon skeleton and the highly defective SSQDs structure enables them to be ideal reactors for electro-redox of CIP. The proposed strategy offers a powerful and feasible way to fabricate SSQDs modified electrode, suggesting potential application of electrochemical sensor for antibiotic.
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Small
·
2023
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IF 13.3
Kai Zhang,Cuiping Xu,Xingjian Zhang,Zhiyi Huang,Qixiang Pian,Kunhong Che,Xiaokun Cui,Yueru Hu,Yimin Xuan
The chemical inertness of CO 2 molecules makes their adsorption and activation on a catalyst surface one of the key challenges in recycling CO 2 into chemical fuels. However, the traditional template synthesis and chemical modification strategies used to tackle this problem face severe structural collapse and modifier deactivation issues during the often-needed post-processing procedure. Herein, a CO 2 self-selective hydrothermal growth strategy is proposed for the synthesis of CeO 2 octahedral nanocrystals that participate in strong physicochemical interactions with CO 2 molecules. The intense affinity for CO 2 molecules persists during successive high-temperature treatments required for Ni deposition. This demonstrates the excellent structural heredity of the CO 2 self-selective CeO 2 nanocrystals, which leads to an outstanding photothermal CH 4 productivity exceeding 9 mmol h -1 m cat -2 and an impressive selectivity of >99%. The excellent performance is correlated with the abundant oxygen vacancies and hydroxyl species on the CeO 2 surface, which create many frustrated Lewis-pair active sites, and the strong interaction between Ni and CeO 2 that promotes the dissociation of H 2 molecules and the spillover of H atoms, thereby greatly benefitting the photothermal CO 2 methanation reaction. This self-selective hydrothermal growth strategy represents a new pathway for the development of effective catalysts for targeted chemical reactions.
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高影响因子
POLYMER COMPOSITES
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2023
·Vol. 44
·期 10
·6440-6453
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IF 5.2
Bi Yang,Beibei Chen,Wenquan Dong,Yang Tong,Jiaye Li
Polymer self-lubricating composite coatings have been widely used on the surface of machinery to extend the life of the moving systems/parts by controlling friction and wear. In this work, epoxy nanocomposite coating with the thickness of about 60 μm was fabricated with addition of hexagonal boron nitride nanosheets (BNNSs)/CeO 2 nanohybrid for enhancement in antifriction and wear resistance. The active BNNSs were first obtained by exfoliating h-BN with alkaline solution, and then the rare earth oxide of CeO 2 nanoparticles were immobilized on the surface of BNNSs through hydrothermal method. The microstructure morphology and chemical composition of as-proposed BNNSs/CeO 2 were characterized by field emission scanning electron microscopy, HRTEM, Fourier transform infrared spectroscopy, RS, X-ray diffraction, and X-ray photoelectron spectroscopy. And the tribological behaviors of epoxy nanocomposite coatings containing BNNSs, CeO 2 , and BNNSs/CeO 2 were investigated comparatively using ball-on disc friction tester (MPX-3). And the 440C stainless-steel ball with diameter of 8 mm was used as the counterface material. Tribological tests showed that epoxy-BNNSs/CeO 2 had the best friction and wear reduction properties, and the lowest coefficient of friction and wear rate of epoxy-based composite coating were achieved when the content of BNNSs/CeO 2 was 0.5 wt%, with 84.9% and 96.3% reduction, respectively. Moreover, the effect of sliding conditions on the tribological performance of epoxy-BNNSs/CeO 2 was investigated. The corresponding enhancing mechanisms of BNNSs/CeO 2 were discussed as well.
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APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Dong Liu,Feiyang Hu,Yue Yan,Runping Ye,Xiaohan Chen,Bingying Han,Zhang-Hui Lu,Li Zhou,Gang Feng,Rongbin Zhang
CO oxidation is the primary approach for eliminating CO from incomplete combustion, and the catalytic performance is dependent on the structure of catalysts. Herein, to explore the structure promotion in the CO oxidation reaction, polymethyl methacrylate was synthesized as the hard template to fabricate the three-dimensional ordered microporous (3DOM) Au/CeO 2 and compared the catalytic performance with the Au/CeO 2 rod catalyst. The 3DOM Au/CeO 2 catalyst could realize complete CO oxidation at 90 °C while 110 °C for Au/CeO 2 rod catalyst. The 3DOM Au/CeO 2 catalyst also showed outstanding stability for 60 h reaction. The achieved high performance could be attributed to the pore structures and the better metal-support interaction that facilitates abundant oxygen vacancies . Additionally, the Au distribution and oxygen vacancies promoted by the macropores structures were discovered using a series of characterizations. This work highlights the promotion of oxygen vacancies and metal-support interaction by 3DOM structure in CO oxidation reaction.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
·Vol. 30
·期 27
·70731-70741
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IF 5.8
Lin Ruixi,Li Jiarong,Jing Xuequan,Guo Meina,Ren Guoqing,Qin Haonan,Yao Zhangwei,Wan Yinhua,Song Weijie,Zeng Huifeng,Yang Feifei,Zhao Da,Hu Kang
Adsorption of vanadium from wastewater defends the environment from toxic ions and contributes to recover the valuable metal. However, it is still challenging for the separation of vanadium (V 5+ ) and chromium (Cr 6+ ) because of their similar properties. Herein, a kind of CeO 2 nanorod containing oxygen vacancies is facilely synthesized which displays ultra-high selectivity of V 5+ against various competitive ions (i.e., Fe, Mn, Cr, Ni, Cu, Zn, Ga, Cd, Ba, Pb, Mg, Be, and Co). Moreover, a large separation factor ( SF V/Cr ) of 114,169.14 for the selectivity of V 5+ is achieved at the Cr 6+ /V 5+ ratio of 80 with the trace amount of V 5+ (~ 1 mg/L). The results show that the process of V 5+ uptake is the monolayer homogeneous adsorption and is controlled by external and intraparticle diffusions. In addition, it also shows that V 5+ is reduced to V 3+ and V 4+ and then formation of V–O complexation. This work offers a novel CeO 2 nanorod material for efficient separation of V 5+ and Cr 6+ and also clarifies the mechanism of the V 5+ adsorption on the CeO 2 surface.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Yunqi Yu,Jianting He,Tong Wang,Xinsheng Qiu,Kangcheng Chen,Qin Wu,Daxin Shi,Yaoyuan Zhang,Hansheng Li
Nitrogen-doped carbon nanotubes (N-CNTs) prepared by carbonization of polypyrrole nanotubes (PPy-NTs) are used as supports. Pt–CeO 2 /N-CNTs electrocatalysts are successfully prepared by in-situ growth of Pt and CeO 2 nanoparticles (NPs) via a one-step coupling method of co-deposition and ethylene glycol reduction. Through structural characterization and electrochemical tests of the prepared electrocatalysts, the effects of preparation conditions on the structure of the electrocatalysts and their electrocatalytic activity for methanol oxidation were systematically investigated. The results verify that the Pt–CeO 2 /N-CNTs electrocatalysts were prepared using N-CNTs calcined at 700 °C as a support and 15 mM alkali concentration. They have the largest electrochemical active area and methanol oxidation mass activity of 85 m 2 g −1 (Pt) and 722 A g −1 (Pt), respectively. Furthermore, the electrochemical stability and anti-CO poisoning performance of the electrocatalysts are significantly better than those of the commercial Pt/C electrocatalysts. The highly-dispersed Pt and CeO 2 in Pt–CeO 2 /N-CNTs, a large number of N sites, and the synergistic action of Pt, CeO 2 , and N-CNTs result in a catalyst with excellent electrocatalytic activity, stability, and resistance to CO poisoning. The support structure and the dispersion of Pt and CeO 2 can be controlled by changing the preparation conditions, which provides a basis for the industrial application of direct methanol fuel cells.
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DALTON TRANSACTIONS
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2023
·Vol. 52
·期 27
·9456-9464
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IF 4
Xiu He,ZhenZhen Mo,Huiling Liu,Cheng Wang
The synthesis of furan-based platform chemicals from abundant and renewable biomass-based hexoses plays an important role in the development and utilization of biomass energy. The electrochemical 5-hydroxymethylfurfural oxidation reaction (HMFOR) represents a promising route for synthesizing the 2,5-furandicarboxylic acid (FDCA) product which is a high value-added biomass-based monomer. Interface engineering is an effective strategy to adjust the electronic structure, optimize the adsorption of intermediates, and expose more active sites, thus attracting extensive attention for designing efficient HMFOR electrocatalysts. Herein, a NiO/CeO2@NF heterostructure with an abundant interface is designed for boosting the HMFOR performance under alkaline conditions. At 1.475 V vs. RHE, the conversion of HMF is nearly 100%, the selectivity of FDCA is 99.0%, and the faradaic efficiency is as high as 98.96%. The NiO/CeO2@NF electrocatalyst also exhibits robust stability for HMFOR for 10 cycles. When coupled with the cathode hydrogen evolution reaction (HER) in alkaline medium, the yields of FDCA and hydrogen production are 197.92 and 600 μmol cm−2 h−1, respectively. The NiO/CeO2@NF catalyst is also suitable for the electrocatalytic oxidation of other biomass-derived platform compounds. The abundant interface between NiO and CeO2, which can regulate the electronic properties of Ce and Ni atoms, improve the oxidation state of Ni species, regulate intermediate adsorption, and promote electron/charge transfer, makes the most contribution to high HMFOR performance. This work will provide a simple route for the design of heterostructured materials and reveal the application prospect of interface engineering for promoting the upgrading of biomass derivatives.
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