ChemCatChem
·
2023
·Vol. 15
·期 7
·e202300194
·
IF 4.5
Tao Li,Mengling Dong,Jiacheng Xu,Tiantian Zhang,Yan Sun,Ning Li,Zuliang Wu,Jing Li,Erhao Gao,Jiali Zhu,Shuiliang Yao,Yong Huang
Graphical CeO 2 /γ-Al 2 O 3 , Pd/CeO 2 , and Pd/CeO 2 /γ-Al 2 O 3 were used for catalyzing low-concentration CH 4 oxidation . γ-Al 2 O 3 can efficiently promote CH 4 oxidation on Pd/CeO 2 and the formation of bicarbonate that is easily gasified to CO 2 . CeO 2 /γ-Al 2 O 3 , Pd/CeO 2 , and Pd/CeO 2 /γ-Al 2 O 3 were used for catalyzing low-concentration CH 4 oxidation. It was found that nano-sized Pd could obviously promote CH 4 oxidation on CeO 2 /γ-Al 2 O 3 . The interaction between Pd and CeO 2 on γ-Al 2 O 3 resulted in higher ratios of Ce 3+ /(Ce 3+ +Ce 4+ ), Pd 2+ /(Pd 2+ +Pd δ+ ), and O ads /(O ads +O latt ), those benefited the formation of more oxygen vacancies and surface reactive oxygen species for CH 4 oxidation. γ-Al 2 O 3 not only supplied a high surface area and enhanced Pd/CeO 2 dispersion on γ-Al 2 O 3 , but also simulated the formation of bicarbonate, where bicarbonate is easier to gasify to CO 2 than bidentate carbonate that formed on Pd/CeO 2 . Operando diffuse reflectance infrared Fourier transform spectroscopy-mass spectrometer analysis results showed that CH 4 oxidation could occur at a temperature as low as 180 °C due to the reaction with surface reactive OH, this reaction was also accompanied by the formation of bicarbonate. The mechanism of CH 4 oxidation promoted by bicarbonate formation on γ-Al 2 O 3 was proposed.
研究领域:
催化化学
·
环境科学
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DOI
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Lei Wang,Yonggang Sun,Yulong Ma,Min Xu,Juan Zhang,Yingbo Zhu,Jie Ding,Li Zhu,Jing Ma,Wenxin Ji,Liqiong Wang,Yuanyuan Li
Dual activation of molecular and lattice oxygen is an important step in the catalytic oxidation of volatile organic compounds. Herein, CeO 2 was derived from MOF as an electron donor support to develop a co-catalyst with Pt-Pd alloy nanoparticles (Pt-Pd/CeO 2 ). The Prepared Pt-Pd/CeO 2 exhibits excellent catalytic activity towards toluene oxidation, showing a turnover frequency (TOF 0.26 s −1 ) higher than those of Pt/CeO 2 (0.05 s −1 ) and Pd/CeO 2 (0.02 s −1 ). Several in situ experimental techniques and density functional theory calculations have revealed that the introduction of Pd valence electrons can intensify the electronic metal-support interactions (EMSIs) effects of Pt-Pd/CeO 2 catalysts, which can weaken the Ce-O bond, thereby promoting the production and circulation of lattice oxygen and oxygen vacancies, and modulating the d -band centre to enhance the adsorption and activation of reactants. This study presents a comprehensive investigation of toluene oxidation on alloy-supported catalysts, providing practical guidance for designing reliable catalysts suitable for industrial applications.
研究领域:
催化化学
·
环境科学
·
材料科学
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产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Haiyan Ruan,Shaofang Zhang,Hongguang Wang,Jiahui Pei,Ruoli Zhao,Xiaoyu Mu,Hao Wang,Xiaodong Zhang
The construction of nanozymes at the atomic level that hold structural stability and high enzyme-like activity is now a key factor in the optimization of an artificial enzyme. Single-atom metal/cerium oxide (CeO2)-based nanozymes have been demonstrated to possess a variety of enzymatic activities and radical scavenging abilities, which are mainly attributed to the single-atom active site, redox valence states, and abundant defect chemistry. Here, we developed a single-atom Pd/CeO2 nanostructure by aqueous phase synthesis that exhibits the advantages of high yield and good stability. The Pd/CeO2 nanostructure possesses peroxidase (POD), superoxide dismutase (SOD), and catalase (CAT) activities as well as reactive nitrogen species free-radical scavenging activity, exhibiting multienzyme-like activities and stability compared with CeO2 and other metal-based nanozymes. It is worth mentioning that the Pd/CeO2 nanostructure exhibits high POD-mimicking activity with a reaction rate of 0.88 μM/min, about 5 times higher than that of the CeO2 nanozyme. In addition, the CAT-like activity of the Pd/CeO2 nanostructure is excellent, and its scavenging rate of hydrogen peroxide reached nearly 100% at a concentration of 50 ng/μL. The present work shows that single-atom Pd substitution is a promising strategy for the design of CeO2 nanozymes to exert better effects on biomedical applications, especially with diseases related to oxidative stress.
研究领域:
纳米技术
·
生物化学
·
材料科学
·
生物医学工程
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DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 67
·38641-38647
·
IF 2.936
Tianyu Guo,Xiaorong Nie,Jianping Du,Jinping Li
A series of Pd/CeO2-nanorods catalysts modified with alkaline-earth metals were prepared by the incipient impregnation method. Their catalytic properties in low-concentration methane oxidation were also investigated. The catalysts were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy and H2-temperature-programmed reduction techniques. The catalytic results show that the Ca element doped in Pd/CeO2, with optimum molar ratio of Pd to Ca of 2 and calcination temperature of 450 °C, improved the properties of the Pd-based catalyst remarkably, which is attributed to strong Pd–support interaction and high oxygen mobility. Therefore, calcium is more suitable as a promoter for enhancing the activities of the Pd/CeO2 catalyst in methane oxidation.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF AEROSOL SCIENCE
·
2016
·
IF 2.278
Nafeng Wang,Shuiqing Li,Yichen Zong,Qiang Yao
Dispersed palladium on the high-surface-area ceria support is synthesized via one-step flame-assisted spray pyrolysis method, which applies a highly-quenched stagnation-point flame controlling catalyst sizes and structures. The X-ray photoelectron spectroscopy (XPS) spectra of Pd show a significantly high binding energy for flame-made Pd/CeO 2 catalysts, possessing a value of 1.7 eV larger than the reference value in literature. It suggests that the partial electron transfer occurs from metal Pd to their supports during the synthesis process, which creates Pd electron-deficient (cationic Pd δ+ ) and Ce electron-rich (anion Ce δ − ), respectively. The catalytic activities of CH 4 oxidation are performed over the temperatures ranging from 200 °C to 600 °C. In comparison with inert support materials, the synergistic effect is found between palladium and support ceria that leads to the enhanced catalytic activity. During the heating and cooling cycles of CH 4 oxidation, Pd/CeO 2 catalysts exhibit an exceptional inhibition effect against the sintering of Pd cluster and its dispersion decrement, which is related to strong electronic interaction of metal-support interfaces induced by the aforementioned partial electron transfer.
研究领域:
催化化学
·
材料科学
·
纳米科技
·
环境催化
·
能源化学
·
表面科学
✓ 已验证
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Zhongchun Yuan,Tingting Cao,Min Deng,Jun Ma,Shuo Geng,Chunliang Yang,Yuan Ren,Mengqin Yao,Fei Liu,Xiaodan Wang
It is very crucial but still a huge challenge to develop efficient and durable catalysts to promote hydrogen production from formic acid (FA). Herein, three CeO 2 with structurally well-defined different shapes, i.e., sCeO 2 (spheres), rCeO 2 (rod) and oCeO 2 (octahedral), are prepared, and their effect on the crystal faces and oxygen vacancy over the constructed heterostructure catalysts (Pd-CeO 2 /C) have been intensively investigated in the FA dehydrogenation. Pd-sCeO 2 /C outperforms the other catalysts with a turnover frequency (TOF) value of 2691 h −1 and selectivity to hydrogen of 100 % at 30 °C. A synergism between the CeO 2 (1 1 0) facet and more oxygen vacancies is considered to be key to obtaining the high reactivity. Moreover, biomass carbon promotes the dispersion of Pd-CeO 2 heterostructures due to its large specific surface area and causes more defects in the Pd-CeO 2 /C. Combined with in-situ FTIR and density functional theory (DFT), it is speculated that FA is decomposed through formate pathway over the Pd-sCeO 2 /C. This work thus provides a reasonable design and controllable synthesis strategy for the effective application of FA as an available liquid phase hydrogen storage material.
研究领域:
催化
·
材料科学
·
化学工程
·
物理化学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 7
·3087-3096
·
IF 3.288
Gang Li,Peng Sun,Fanggen Wu,Jie Zhao,Dongxue Han,Guofeng Cui
4-Aminophenol (4-AP) is a highly toxic environmental pollutant and contaminant of medicine, which is widely used in industries and daily life. Therefore, the development of a reliable sensor for determining the amount of 4-AP is of great importance for the protection of human and environmental health. Herein, by fabricating a Pd@CeO2 composite on a nanoporous gold-coated carbon fiber paper (NPG/CFP), the sensing properties for 4-AP can be largely enhanced. Combining the significant increase in the catalytic activity of the Pd@CeO2 composite (derived from the strong interactions between Pd and CeO2) with the NPG and NPG/CFP hierarchical porous structure having a high electrochemically active surface area, the electrode achieved excellent detection of 4-AP. It manifested an extremely high sensitivity of 75.4 μA μM−1 and 56.5 μA μM−1 in the concentration range from 0.005 μM to 0.03 μM and 0.03 μM to 9 μM, respectively. The detection limit reached as low as 4 nM under optimized conditions (S/N = 3). The electrode also possesses long-term stability and presents great anti-interference ability. All these results demonstrate that the electrode is a promising candidate for future sensors for monitoring 4-AP in water and pharmaceuticals.
研究领域:
分析化学
·
环境科学
·
材料科学
·
电化学
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产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2025
·
IF 7.2
Jiaman Wang,Jing Xiong,Zekai Cui,Yuanfeng Li,Hao Guo,Guilin Liu,Yaxiao Ma,Linsheng Xu,Jinqing Jiao,Jianping Zou,Yuechang Wei
CeO 2 , a pivotal rare earth oxide in environmental catalysis, has garnered extensive interest for soot oxidation owing to its exceptional oxygen storage capacity and oxygen vacancy-rich surfaces. To further optimize catalytic efficiency, we engineered spherical CeO 2 with exposed (111) facets via hydrothermal synthesis and uniformly anchored Pd species through a gas bubbling-assisted membrane reduction (GBMR) strategy. The formation of Pd–O–Ce interfacial units is identified as critical active sites, where metal-support interaction (MSI) significantly enhances oxygen transfer. Notably, the Pd 1.0 /CeO 2 catalyst achieves a remarkable T 50 of 356 °C (14% lower than pristine CeO 2 ), attributed to highly dispersed Pd species and abundant Pd–O–Ce interfaces. In contrast, excessive Pd species loading induces particle agglomeration, weakening MSI effect and catalytic performance. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional thoery (DFT) calculations reveal that the Pd–O–Ce interface promotes NO adsorption – the rate limiting step – by generating electron-rich Pd sites and oxygen vacancies, thereby accelerating NO-to-NO 2 conversion and subsequent soot oxidation. This work highlights the pivotal role of interfacial engineering in optimizing Pd–CeO 2 catalysts, offering a rational design strategy for high-performance soot oxidation systems in diesel emission control.
研究领域:
环境催化
·
材料科学
·
多相催化
·
排放控制
·
纳米材料
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2023
·Vol. 25
·期 13
·5150-5159
·
IF 9.8
Yuzhen Hu,Yanbin Cui,Shuoxiao Zhao,Xuelai Zhao,Xiaohong Hu,Zhenlong Song,Wei Fan,Qi Zhang
Selective cleavage of C–C bonds in the lignin structure is crucial for the depolymerization of lignin and producing value-added chemicals. In this study, we reported that Pd/CeO2 catalysts can selectively catalyze the Cα–Cβ bond cleavage of oxidized lignin model components and authentic lignin in an aqueous phase under mild conditions (50 °C, ambient pressure). A variety of β-O-4 and β-1 ketones with representative Cα–Cβ bonds were successfully cleaved yielding aromatic acids and phenols in 76.8–94.9% yields. Their unique catalytic properties are derived from the electron transfer between Pd and CeO2 support which facilitates active Pd2+ sites and reactive oxygen species formation. A mechanistic study elucidates that base-mediated C–H bond activation via enolization and in situ reactive oxygen species (˙O2−) formation are the key steps for the selective Cα–Cβ cleavage. Furthermore, the applicability of the system for the bond cleavage in an authentic lignin sample was demonstrated. Nearly 54.2 wt% of oxidized bamboo lignin was converted, generating aromatic monomer yields up to 35.9 wt%, with a high selectivity for aromatic aldehydes.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2026
·Vol. 9
·期 30
·14592-14602
·
IF 5.8
Mu Yueru,Lian Rui,Zhang Jingjing
Silver ions (Ag + ) pose significant ecological
and health
risks due to their toxicity and potential for bioaccumulation. While
conventional detection methods such as ICP-MS and AAS offer high sensitivity,
they are often hindered by complex operations, high costs, and limited
suitability for on-site analysis. To address this, we developed a
highly active and selective colorimetric sensor for Ag + based on a DNA-encoded Pd/DNA/CeO 2 nanozyme. Cerium oxide
nanorods (CeO 2 ) serve as an effective support for the directional
immobilization of single-stranded DNA through phosphate-Ce 4+ coordination and electrostatic interactions. The DNA template guides
the uniform in situ growth of palladium nanoparticles (Pd NPs), forming
a well-dispersed and highly exposed catalytic interface. The resulting
Pd/DNA/CeO 2 nanozyme exhibits enhanced peroxidase-like
activity, catalyzing the oxidation of 3,3 ′ ,5,5 ′ -tetramethylbenzidine
(TMB) in the presence of H 2 O 2 . Ag + ions are specifically reduced on the Pd surface to form a metallic
Ag layer, which effectively blocks the active sites and quenches the
catalytic activity, enabling a “switch-off” detection
mode. The optimized sensor shows a wide linear response to Ag + from 50 to 400 nM with a detection limit of 22.7 nM. It also
demonstrates excellent selectivity against common interfering ions
and good applicability in real water samples. This DNA-encoded nanozyme
design provides a robust and facile platform for the on-site monitoring
of trace Ag + in environmental systems.
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 48
·18562-18571
·
IF 4.569
Han Zhao,Longchun Bian,Junchen Du,Yunkun Zhao
The Pd distribution and the CeO2–Al2O3 combination are among the decisive factors for the performance of commercial three-way catalysts. Generally, the sufficient doping of Pd into ceria-based oxides and the intimate interaction between CeO2 and Al2O3 could both benefit the three-way catalytic reactions. However, in the present work, the moderate doping of Pd into CeO2 and less intimate CeO2–Al2O3 interaction were found to be responsible for the much higher catalytic activity (the decrease in T50 was 52, 119, or 55 °C for C3H6, CO, or NO) in PdCe/Al2O3-CP than PdCe/Al2O3-Imp, for which the Pd and Ce species were co-loaded onto Al2O3 through the co-precipitation or impregnation method, respectively. It was intriguing to find that the co-precipitated PdCeOx in PdCe/Al2O3-CP showed less sufficient doping of Pd into CeO2 than the co-impregnated PdCeOx in PdCe/Al2O3-Imp; as a result, both a higher fraction of highly active metallic Pd and a higher Pd dispersion were realized in PdCe/Al2O3-CP. Moreover, due to the less intimate CeO2–Al2O3 interaction, specifically the less severe penetration of the Pd and Ce species into Al2O3, PdCe/Al2O3-CP showed higher Pd dispersion, specific surface area, pore volume and size than PdCe/Al2O3-Imp. The presence of more abundant reactive Pd0, and the higher accessibility of the active Pd and CeO2 sites, together with improved redox properties and enriched oxygen vacancies contributed much to the enhanced three-way catalytic activity of PdCe/Al2O3-CP. Additionally, simultaneously optimizing the Pd distribution and the CeO2–Al2O3 combination in a single step, as reported in this work, is also highly desirable in industry.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 15
·4489-4497
·
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
·
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）