Molecular Catalysis
·
2021
·
IF 5.062
Hanlin Huang,Jiajun Dai,Xiaobin Liu,Kok Bing Tan,Jiale Huang,Guowu Zhan,Qingbiao Li
In recent years, high value utilization of waste biomass has been a hot topic in scientific research. Herein, waste eggshell (ES) rich in sulfonic groups was utilized as a natural modified support to load Pd and Ag nanoparticles (NPs), leading to efficient Pd-Ag/ES catalysts for the catalytic hydrogenation of 1,3-butadiene. Through series of characterizations such as SEM, TEM, BET, XPS, and FTIR, it was found that the porous ES not only has hierarchical structures to facilitate the metal dispersion, but also interacts strongly with Pd and Ag NPs via the inherent surface sulfonic groups, which are responsible for the enhanced catalytic performance. The optimized Pd-Ag/ES catalyst exhibited butenes selectivity of 95.8% and 1,3-butadiene conversion of 95% at 45 °C with excellent stability for at least 30 h on-stream. Furthermore, the first-principles density functional theory (DFT) calculation and in situ DRIFTS were performed to explore the plausible mechanism underlying the enhanced catalytic performance due to sulfonic groups. It is suggested that the sulfonic groups can effectively reduce the adsorption energy of butenes and 1,3-butadiene on the surface of Pd NPs which are beneficial to the selectivity of butenes. This work exemplifies that the waste ES with inherent sulfonic groups can be used as excellent support materials for loading active metal nanoparticles for selective hydrogenation reactions. Collectively, we verified that biological waste like eggshell has a great potential in serving as catalyst carrier due to its unique advantages.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 48
·27320-27331
·
IF 12.732
Pengcheng Wu,Hui Liu,Mengqi Sun,Yaxin Zeng,Jiawei Ye,Song Qin,Yimin Cai,Wen Feng,Lihua Yuan
Efficient palladium recovery from high level liquid wastes (HLLW) is of increasing priority for sustainable development and addressing issues in radioactive waste treatment. However, searching for robust materials for palladium sorption, in the presence of large amounts of competing ions even at rather high acidity still poses a great challenge. Herein we present two novel cationic covalent triazine frameworks (denoted as CTF-S and CTF-L) created by polymerization of monomers IL-S and IL-L for palladium recovery. The resultant CTF-S and CTF-L with respective surface areas of 212.9 m2 g−1 and 342.5 m2 g−1 exhibit excellent sorption ability toward palladium at high acidity. This has been demonstrated by a maximum sorption capacity of 333 mg g−1, which is the highest at 3 M HNO3 among all porous adsorbents reported so far. More importantly, these materials reveal remarkable selectivity toward palladium over other metal ions that are co-existing in simulated HLLW. In addition, thanks to the relatively large π-conjugated structures, no obvious decrease in sorption capability was observed after being exposed to 1000 kGy γ irradiation. Desorption could be easily achieved by a single contact with a mixed solution of 1 M thiourea and 1 M HCl and the sorption performance still remains at the initial level without conspicuous loss after five cycles. The XPS results, anion competitive experiments, and DFT calculations propose a sorption mechanism in which the anion exchange between anionic Pd complexes and chloride, and the chemical coordination between triazine N and Pd(II) work coorperatively to enhance the sorption capacity. This work not only provides a new kind of excellent adsorbent for selective palladium recovery, but also demonstrates a promising approach for constructing robust materials for nuclear waste remediation.
研究领域:
材料科学
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核化学与放射化学
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环境科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2025
·
IF 4.7
Yanni Wang,Yuan Tian,Jiahao Ma,Xiuping Ding,Yabin Wang
To effectively improve performances of silica-based supported catalysts against the aggregation and leaching of anchored metal nanoparticles, functional interfaces have been naturally introduced between SiO 2 substrates and active matters. Regrettably, when mono-, di- and tri-aminosilanes are utilized as interfacial functional layers, their influences on physicochemical properties and catalytic performances of target catalysts have not been contrasted and revealed up to now. In this work, we attempt to explore these effects by selecting commercial aminosilanes with variable aminoalkyl chains inside (mono-, di- and tri-amino groups as 1 N, 2 N, and 3 N) and dendritic mesoporous silica nanoparticles (DMSNs) as supports. Three types of DMSNs-supported palladium catalysts have been conceived, including DMSNs-1N-Pd, DMSNs-2N-Pd, and DMSNs-3N-Pd. Their morphologies, architectures, compositions of crystal phases, surface functional groups, and loading contents of Pd have been compared and the differences have been accordingly explained. The three materials have potentials to function as photocatalysts. Moreover, catalytical performances have been evaluated by Pd-catalyzed Suzuki coupling reaction as the model to reveal the interfacial effects of 1 N, 2 N, and 3 N. Most importantly, this work can guide researchers to reasonably choose mono-, di- or tri-aminosilane with variable aminoalkyl chain in practical applications.
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
Catalysts
·
2025
·Vol. 15
·期 6
·544
·
IF 4
Tingting Hu,Baozeng Ren,Liang Zhao
Hydrogen peroxide (H2O2) is an important industrial chemical that is widely applied in many areas. The direct synthesis of H2O2from H2and O2has proved to be a green and economic pathway. Pd-based bimetallic catalysts, due to their superior catalytic performances in this reaction, have attracted intensive attention. Herein, Tetrakis(hydroxymethyl)phosphonium chloride (THPC) was adopted as the protective ligand to immobilize Pd-Au alloy nanoparticles onto activated carbon (AC). The varied Pd/Au molar ratios demonstrated homogeneously distributed Pd-Au nanoalloys with average particle sizes ranging from 3.51 to 5.75 nm. The optimal ratio was observed over the Pd3Au1/AC-THPC catalyst with a maximum H2O2productivity of 165 mol/(kgPd·h) and selectivity of 82.3% under ambient pressure. The relationship between the electronic structure and catalytic activity indicated Pd0was the active site, while the presence of Au inhibited H2O2degradation rate. This research could help in the design efficient bimetallic catalysts for the direct synthesis of H2O2.
研究领域:
化学
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
HELVETICA CHIMICA ACTA
·
2022
·Vol. 105
·期 6
·e202200017
·
IF 2.201
Geng-Wei Liu,Peng-Bin Pan,Xin Zhang,Yuan-Yuan Huang,Peng Liu,Ye-Yan Qin,Yuan-Gen Yao
Zinc titanate (ZnTiO 3 ) has recently been applied in various areas for its unique properties. Herein, through tuning the phase structures of ZnTiO 3 support, we synthesized two different Pd-based catalysts for CO oxidative coupling to DMO and further investigated their structure-activity relationships for the first time. The results indicated that the strong metal-support interaction between the cubic phase ZnTiO 3 and Pd species leads to an enriched Pd electronic density and promotes the bridged CO adsorption. As a result, the as-synthesized catalyst with cubic phase ZnTiO 3 performed a turnover frequency (TOF) of 339.3 min −1 , which was much higher than the hexagonal one (226.3 min −1 ).
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Chuanliang Li,Fan Gao,Yangyang Ren,Baosong Li,Lanlan Li,Zunming Lu,Xiaojing Yang,Xinghua Zhang,Xiaofei Yu
Metallic ultrathin nanosheets have drawn increasing attention due to their distinct properties and wide applications. Nonetheless, the successful preparation of metallic ultrathin nanosheets is still a huge challenge because metallic bonds have no direction and tend to form three-dimensional close-packed structures. Here, ultrathin curved PtPdMo nanosheets (UC-PtPdMo NSs) were obtained by controlling the anisotropic growth kinetics through the CO released from Mo(CO)6. Meanwhile, different doses of PVP and CTAB could induce the formation of ultrathin porous PtPdMo NSs (UP-PtPdMo NSs) and ultrathin PtPdMo NSs (U-PtPdMo NSs). Among them, UC-PtPdMo NSs had the optimal catalytic activity for oxygen reduction reaction (ORR), and its specific and mass activities were 4.1 and 3.6 times as large as those of Pt/C. Moreover, it showed better stability than the other catalysts after 10k cycles. The strengthened catalytic properties might have resulted from the ultrathin structures and the electronic adjustment of Pt by Pd and Mo elements.
研究领域:
材料科学
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化学
✓ 已验证
DOI
高影响因子
Chemistry-An Asian Journal
·
2021
·Vol. 16
·期 22
·3743-3747
·
IF 4.568
Min-Jie Chen,Gang-Gang Chang,Li-Yan Chen,Ke-Xin Huang,Chun Pu,Dan Li,Yao Yao,Jia-Xin Li,Xiao-Yu Yang,Banglin Chen
Graphical The core-shell catalyst with surface wrinkles greatly improves the selectivity of tandem catalysis. Process intensification, targeting the maximization of spatial-temporal productivity utilizing minimum energy and resources has always been the constant trends especially in chemical industry. In this regard, tandem reactions that are able to perform a multi-step reaction in a single pot by eliminating costly separation steps have been viewed as a typical paradigm. However, a spatial isolation of varied active sites with a controlled manner in a single catalyst to avoid deactivation and work synergistically is a challenging problem yet sometimes being overlooked. In this work, a spatial base-metal core-shell structured catalyst with wrinkled surface was successfully fabricated by a direct homoepitaxial growth method in an acid/water system, which exhibited increased hydrophobicity, exposure of active sites and significantly improved product selectivity towards one-pot Knoevenagel condensation-hydrogenation tandem reaction compared with the uncoated catalyst. Meanwhile, the catalytic performance was largely retained and the structural stability was maintained even after successive 8 cycles, which shows great promise for industrial applications.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2019
·Vol. 33
·期 11
·e5198
·
IF 3.259
Yu Ru,Yanli Huang,Yuanyuan Wang,Liyi Dai
Well distributed Pd-Cu bimetallic alloy nanoparticles supported on amine-terminated ionic liquid functional three-dimensional graphene (3D IL-rGO/Pd-Cu) as an efficient catalyst for Suzuki cross-coupling reaction has been prepared via a facile synthetic method. The introduction of IL-NH 2 cations on the surface of graphene sheets can effectively avoid the re-deposition of graphene sheets, allowing the catalyst to be reused up to 10 cycles. The addition of Cu not only saves cost but also ensures high catalytic efficiency. It is worthy to note that the catalyst 3D IL-rGO/Pd 2.5 Cu 2.5 can efficiently catalyze the Suzuki cross-coupling reaction with the yield up to 100% in 0.25 h, almost one-fold higher than that by the pristine IL-rGO/Pd 2.5 catalyst (52%). The Powder X-Ray Diffraction (XRD), combining energy dispersive X-ray spectroscopy (EDS) mapping results confirm the existence and distribution of Pd and Cu in the bimetallic nanoparticles. The transmission electron microscopy (TEM) reveals the nanoparticle size with an average diameter of 3.0 ± 0.5 nm. X-ray photoelectron spectroscopy (XPS) analysis proved the presence of electron transfer from Cu to Pd upon alloying. Such alloying-induced electronic modification of Pd-Cu alloy and 3D ionic liquid functional graphene with large specific surface area both accounted for the catalytic enhancement.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Tianshuang Wang,Inci Can,Sufang Zhang,Junming He,Peng Sun,Fangmeng Liu,Geyu Lu
The design of semiconductor metal oxides (SMOs) with well-ordered porous structure has attracted tremendous attention owing to their larger specific surface area. Herein, three-dimensional inverse opal In2O3 microspheres (3D-IO In2O3 MSs) were fabricated through one-step ultrasonic spray pyrolysis (USP) which employed self-assembly sulfonated polystyrene (S-PS) spheres as a sacrificial template. The spherical pores observed in the 3D-IO In2O3 MSs had diameters of about 4 and 80 nm. Subsequently, the catalytic palladium oxide nanoparticles (PdO NPs) were loaded on 3D-IO In2O3 MSs via a simple impregnation method, and their gas sensing properties were investigated. In a comparison with pristine 3D-IO In2O3 MSs, the 3D-IO PdO@In2O3 MSs exhibited a 3.9 times higher response (Rair/Rgas = 50.9) to 100 ppm acetone at 250 °C and a good acetone selectivity. The detection limit for acetone could extend down to ppb level. Furthermore, the 3D-IO PdO@In2O3 MSs-based sensor also possess good long-term stability. The extraordinary sensing performance can be attributed to the novel 3D periodic porous structure, highly three-dimensional interconnection, larger specific surface area, size-tunable (meso- and macroscale) bimodal pores, and PdO NP catalysts.
研究领域:
材料科学
·
化学传感
·
纳米技术
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2018
·
IF 4.7
Jianzhou Wu,Hehe Qian,Linfang Lu,Jie Fan,Yongsheng Guo,Wenjun Fang
A facile synthesis strategy has been developed to synthesize palladium nanocubes with tunable size and well-controlled morphology. Through adjusting the dosages of acetate species (KOAc, NH4OAc, and HOAc), the sizes of well-defined Pd nanocubes are tuned. The reduction of Pd precursors, a first-order reaction, is influenceable by acetate species, and a quantitative relationship between cubic width and apparent reduction rate constant, which has been found to be an effective parameter to describe the growth process of Pd nanocubes, has been uncovered. The effect of apparent reduction rate constant on the growth of Pd nanocubes has been discussed, and the growth kinetics of Pd nanocubes is quantitatively depicted.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Applied Catalysis O: Open
·
2024
·
IF 0
Zhe Zhang,Weiting Xiao,Yufei He,Dianqing Li,Xiaodong Zhao
During the manufacture of Al 2 O 3 , sulfate would be inevitably introduced when aluminum sulfate is used as raw material, but its effect has received little attention. In this work, Al 2 O 3 supports with different sulfate content were synthesized and used to prepare Pd/Al 2 O 3 catalyst. Sulfates in all samples exist as surface sulfate, and would be partially removed during the preparation process. Sulfate existing in Al 2 O 3 supports had little impact on the electric structure of Pd, but would partially block pores and also consume surface hydroxyl groups. As a result, higher sulfate content in support would lead to lower Pd dispersion in catalysts and slower reaction rate towards the hydrogenation of amyl-anthraquinone.
研究领域:
材料科学
·
催化化学
·
物理化学
✓ 已验证
DOI
ChemistrySelect
·
2024
·Vol. 9
·期 47
·e202404091
·
IF 1.9
Rui Wang,Jiali Yuan,Huan Zhang,Xiang Liu,Jiani He,Lihua Zhu
Graphical Th Pd/NC catalysts with different Pd loadings were synthesized via sodium borohydride liquid-phase reduction method. Among of the catalysts, 2.52%Pd/NC catalyst exhibits the best performance and high stability in the 4-nitrophenol hydrogenation reaction with TOF = 321.8 h −1 and 100% selectivity at high conversion of 4-nitrophenol. A series of the Pd/NC samples with various Pd loadings (0.11%, 0.48%, and 2.52%) are prepared via sodium borohydride (NaBH 4 ) reduction method and carbon doping with nitrogen (NC) is acquired by the pyrolysis of ZIF-8. The samples are characterized by XRD, BET, SEM, TEM, HRTEM, STEM-EDX elemental maps and line-scanning, XPS, TG, and so forth. It confirms that the Pd nanoparticles (NPs) are successfully coated on the NC. The catalytic behaviors of the samples are evaluated by the hydrogenation of 4-nitrophenol (4-NP), the 2.52%Pd/NC catalyst shows the best catalytic property among as-obtained catalysts maybe due to the much more Pd(0) species. The 2.52%Pd/NC catalyst exhibits 100% selectivity to 4-aminophenol (4-AP) at high conversion of 4-nitrophenol and 321.8 h −1 turnover frequency (TOF) under mild reaction conditions (3.0 MPa H 2 , 40 °C, 1 h). Moreover, the catalysts show an excellent stability.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）