NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 8
·3573-3580
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IF 2.7
Ruidong Li,Bo Zhao,Ganggang Chang,Shanchao Ke,Minjie Chen,Didi Dong,Chun Pu,Xiaoyu Yang
In the current investigation, the base-metal hollow multifunctional catalyst, Pd–IL@H-UiO-66-NH2, was fabricated utilizing a hydrothermal method followed by etching and supporting processes. The results of the effort demonstrate that Pd–IL@H-UiO-66-NH2 displays significantly enhanced activity and product selectivity in catalysis of the one-pot Knoevenagel condensation–hydrogenation reaction, as well as a high level of generality in promoting hydrogenation reactions of unsaturated hydrocarbons. The excellent properties of Pd–IL@H-UiO-66-NH2 are ascribed to its rationally designed spatial distribution of catalytically active sites within its hierarchical structure, which is comprised of surface wrinkles that increase hydrophobicity and exposure of the active sites, and hollow structures that serve as nanoreactors to enrich substrate interactions and improve mass transfer. Furthermore, the catalytic stability of Pd–IL@H-UiO-66-NH2 was shown to be largely maintained after its use in five successive catalytic cycles. The stability of the new tandem catalyst benefits from strong confinement effects associated with its hollow structure and electronic interactions between the Pd and ILs that effectively restrict leaching and aggregation of Pd nanoparticles (NPs).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Bowen Wang,Lu Song,Chen Peng,Ximeng Lv,Gengfeng Zheng
The acidic CO 2 reduction reaction (CO 2 RR) offers a promising approach to mitigate CO 2 reactant loss and carbonate deposition, which are challenging issues in alkaline or neutral electrolytes. However, the hydrogen evolution reaction (HER) competes in the proton-rich environment near the catalyst surface as a side reaction, reducing the energy efficiency of generating multi-carbon (C 2+ ) products. In this work, we proposed a palladium (Pd) doping strategy in a copper (Cu)-based catalyst to stabilize polarized Cu 0 -Cu + sites, thus enhancing the C C coupling step during the CO 2 RR while suppressing HER. At an optimal doping ratio of 6%, the Pd dopants were well dispersed as single atoms without aggregation, allowing for the stabilization of subsurface oxygen (O Sub ), preserving the polarized Cu 0 -Cu + active sites, and reducing the energy barrier of C C coupling. The Pd-doped Cu/Cu 2 O catalyst exhibited a peak Faradaic efficiency (FE) of 64.0% for C 2+ products with a corresponding C 2+ partial current density of 407.1 mA∙cm −2 at −2.18 V versus a reversible hydrogen electrode, a high CO 2 single-pass conversion efficiency (SPCE) of 73.2%, as well as a high electrochemical stability of ∼ 150 h at industrially relevant current densities, thus suggesting a potential approach for tuning the electrocatalytic CO 2 performances in acidic environments with higher carbon conversion efficiencies.
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CRYSTENGCOMM
·
2024
·Vol. 26
·期 27
·3609-3626
·
IF 2.6
Jie Jin,Haoran Li,Shanshan Wu,Jing Wang,Qunling Fang,Chunyan Xu,Yunqi Xu,Weili Kong,Di Wang,Shouhu Xuan
With the rapid development of social industrialization, energy crisis and environmental problems are becoming increasingly serious. Therefore, there is an urgent need to synthesize multi-mode nanocatalysts for general application. In this paper, a h-Fe3O4@Pd/PDA nanocatalyst with Pd nanocrystals sandwiched between a h-Fe3O4 hollow sphere and a polydopamine (PDA) shell was prepared by a simple redox-oxidative polymerization method. The catalytic activity of h-Fe3O4@Pd/PDA hollow spheres was evaluated using selective reduction hydrogenation of 4-nitrostyrene, reduction of 4-nitrophenol and oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) as catalytic models. h-Fe3O4@Pd/PDA has reduction kinetics of 4-nitrophenol up to 0.77 min−1 mg−1. Importantly, the rate of 4-nitrophenol reduction catalyzed by h-Fe3O4@Pd/PDA was enhanced by 1.43 times under near infrared light (NIR, 808 nm) irradiation. In addition, NIR laser can induce the selective reduction of 4-nitrostyrene to 4-aminostyrene by h-Fe3O4@Pd/PDA with a selectivity of 84.8%. Under different reaction scenarios, h-Fe3O4@Pd/PDA hollow spheres could be recycled by magnetic recovery, and the catalytic reaction activity was above 70% after six cycles. As a result, owing to the simple fabrication, good magnetic separation and high NIR-enhanced catalytic properties, h-Fe3O4@Pd/PDA exhibited a wide range of potential in nanocatalysis.
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Small
·
2024
·Vol. 20
·期 52
·2408373
·
IF 13
Xiaotong Zhou,Songliang Liu,Huaifang Teng,Kun Ma,Weixin Miao,Xuejing Cui,Xin Zhou,Luhua Jiang
Reasonable construction of high activity and selectivity electrocatalysts is crucial to achieve efficient ethanol oxidation reaction (EOR). However, the oxidation of ethanol tends to produce CO species that poison the active centers of the EOR electrocatalysts. Herein, a unique amorphous CrO x -protected defect-rich ultrafine Pd nanowires (CrO x -Pd NWs) is developed. On the one hand, the CrO x layer can act as a protective layer to maintain the structure of the nanowire. On the other hand, it can play the role of OH regulator to optimize the adsorption energy barrier of intermediate species in Pd nanowire, thereby enhancing the ability of the catalyst to resist CO poisoning. The CrO x -Pd NWs exhibit excellent EOR performance with 3.64 times higher mass activity and 50 mV lower CO electro-oxidation potential than commercial Pd black. The results show that the CrO x layer promotes the dissociation of H 2 O into OH ads , while the CrO x transfers electrons to neighboring Pd atoms optimizing the electronic configuration of Pd, thus selectively oxidizing ethanol to acetate and preventing the formation of toxic * CO. This work provides an effective strategy for the synthesis of nanowire materials with oxide/metal interfaces and offers new ideas for the design of catalysts that can efficiently drive EOR.
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JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Qiang Zhou,Xinyu Wang,Tao Xing,Mingqing Wang,Mingbo Wu,Wenting Wu
Hydrogen peroxide (H 2 O 2 ) is widely used as an oxidant for photocatalytic oxidation of methane to value-added chemicals under mild conditions, but suffers from low utilization efficiency. Herein, we propose a comprehensive strategy for the proper amount of hydroxyl radicals (•OH) generation from H 2 O 2 by regulating the Pd/Au molar ratios and the total Au-Pd contents loaded on In 2 O 3 . For the photocatalytic oxidation of methane at ambient temperature, the yield and selectivity of CH 3 OH over the optimized 1.0% AuPd 0.5 /In 2 O 3 catalyst were as high as 2187.0 μmol g −1 h −1 and 94.0% respectively, exceeding most reported literatures. Mechanism investigations revealed that the formation of Au-Pd alloys may contribute to the homolytic cleavage of H 2 O 2 into •OH radicals and improve the selectivity of •OH generation. This work provides some guidance for the delicate design of photocatalysts to manipulate selective H 2 O 2 activation and efficient photocatalytic methane oxidation.
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Molecular Catalysis
·
2025
·
IF 4.9
Bo Jiang,Shu-Lin Liu,Zhe-Yan Jin,Zhao Wang,Bin-Can Cheng,Ze-Long Guan,Ying Hong,Zhao Wei,Zhi Qiao,Jian Tao,Bao-Lian Su
Selective hydrogenation driven by heat is a critical industrial process for purifying alkene feedstocks with serious problems of energy and H 2 consumption. Photochemistry-assisted strategy offers a sustainable alternative owing to its superiority of H 2 -free reaction under ambient temperature, unfortunately, with a challenging demand on efficient catalysts. Herein, a wide-spectrum-responsive Pd/N-TiO 2 photo-thermal catalyst was developed by a solvothermal method for photochemistry-assisted selective hydrogenation of butadiene in propene. It shows an excellent catalytic performance, with 100 % alkenes selectivity and 100 % butadiene conversion under irradiation of full-light (i.e., 320 nm∼780 nm). Notably, over 53 % butadiene conversion with 100 % alkenes selectivity was successfully retained on Pd/N-TiO 2 after shortening the wavelength range to visible light, much superior to that on Pd-TiO 2 (i.e., <1 % butadiene conversion). Further exploration reveals that the nitrogen doping extends the light-responsive wavelength of titanium oxide from ∼380 nm to above 500 nm owing to the formation of Ti 3+ and oxygen vacancies, which later create a defect energy level (i.e., ∼-0.53 to -0.12 eV) between the valence-conduction band of TiO 2 . The wide spectral response of N-TiO 2 enhances the water photolysis to produce intermediate hydrogen ([H]) that acts as the hydrogen source for the tandem butadiene hydrogenation over the Pd surface. The work indicates that developing a dual-functional catalyst with an expanded light-responsive wavelength is an efficient way to enhance the photochemistry-assisted selective hydrogenation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Lu Lin,Yongjian Zeng,Suyu Zhang,Di Hu,Zhiwei Jiang,Guoqing Guan,Kai Yan
The hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF) to biofuel 2,5-dimethylfuran (DMF) serves as a vital reaction in biomass refineries. Herein, Pd-UiO-66 catalysts with controlled contents of ligand-vacancies were developed for the HMF-to-DMF conversion. Strikingly, a volcano-like relationship between defect level and HDO activity was obtained. The DMF yield was promoted ∼3 times, reaching 92.2 % at 160 °C and 15 bar H 2 , which refers to a high-level turnover frequency value of 42.66 h −1 among the reported candidates. The Pd-UiO-66 catalysts also afforded >80 % yield for the HDO of 5-methyl furfural, furfural, and vanillin. Besides, high HDO activity could be retained in five recycles. Manipulating the contents of ligand-vacancies was confirmed to create more Pd 0 species and Bronsted acid sites, leading to remarkable performance. This work provides significant inspiration for tuning structural defects in MOFs to realize the efficient HDO of platform molecules in biomass valorization.
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Molecular Catalysis
·
2024
·
IF 3.9
Zhe Zhang,Jianan Zhang,Shuai Chen,Yanan Liu,Yufei He,Dianqing Li
Hydrogen spillover phenomenon can significantly impact the activity in hydrogenation reaction, but the spillover is limited in a very short range on non-reducible Al 2 O 3 , a most widely used industrial support. Herein, Al 2 O 3 doped with different lanthanides (ln) was prepared by co-precipitation, which was then used to produce Pd/ln-Al 2 O 3 catalysts. These catalysts display much higher hydrogenation activity towards alkylated anthraquinone than undoped Pd/Al 2 O 3 catalyst and those modified by non-lanthanide elements. After the introduction of lanthanides, the reaction order of H 2 decreases from 1 to 0. Further characterization and DFT calculation show that H 2 storage ability is increased for ln-doped catalysts due to the low activation energy of H transfer and low adsorption energy of H on O(-ln) sites. In addition, a reasonable relationship between reducibility of ln 3+ in catalysts and the catalytic performance is found.
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Materials Today Chemistry
·
2025
·
IF 6.7
Tianwei Wang,Hua Lin,Zhicheng Tang,Rongwen Lu,Shufen Zhang
The hydrogenation of furfural (FFA) to tetrahydrofurfuryl alcohol (THFOL) is of immense commercial significance. This transformation, however, remains challenging and often requires high temperature and pressure to achieve high selectivity, or more importantly, the design and development of novel catalysts. Herein, we develop the rattle-typ (Pd@HASs) nanoreactors for selective hydrogenation of FFA to tetrahydrofurfuryl alcohol at mild condition via a regulatable metal-doped vesicles method, which was assembled from the double hydrophobic anionic surfactant AOT (sodium dioctyl sulfosuccinate). The structure and growth process of the Pd@HASs were analyzed by HRTEM, SEM, XPS and DLS. Through the regulation means which modulated the metal coordination or anionic environment, the metal-doped vesicles with tunable size and distribution of metal nanoparticles could convert to a series of Pd@HASs with different cavity sizes from 32 nm to 144 nm. The Pd@HASs exhibited great selectivity in FFA hydrogenation, with a tetrahydrofurfuryl alcohol yield of >99 % within an hour at 120 °C, 10 bar H 2 pressure. Among the nanoreactors with different cavity sizes, Pd@HASs with a 50 nm cavity has the best performance. This work provides a new way for the design and synthesis of hollow alumina nanospheres encapsulated metal nanoparticles nanoreactors, and the selective hydrogenation of FFA at mild condition.
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FOOD CHEMISTRY
·
2025
·
IF 9.8
Zhiwei Zhu,Shuqi Huang,Da-Wen Sun
The monitoring of ethylene continues to pose significant challenges for conventional sensors, primarily due to their instability when subjected to environmental fluctuations. Consequently, in the study, a coordination-stabilized Pd(II)/His@SiO 2 nanocomposite was engineered through the optimization of the histidine (His)-Pd(II) molar ratio (Pd-His-1-0.8). This was achieved by suppressing the hydrolysis/thermal decomposition of Pd(NO 3 ) 2 to ensure uniform dispersion of Pd(II) via His-SiO 2 hydrogen bonding. A 4 × 4 colourimetric sensor array, based on the Pd-His-1-0.8 and integrated with pH-responsive dyes, was constructed. This array generated unique fingerprints mediated by the Wacker reaction, facilitating the quantification of ethylene. The stability experiment proved that the sensor exhibited negligible signal drift across harsh conditions (25–70 °C, 43–81 % RH) and 21 d storage. Furthermore, some postharvest storage experiments using bananas as a representative fruit demonstrated that results obtained from the colourimetric sensor array were in good agreement with those from commercial detectors. This indicates the considerable potential of the sensors for applications in food and agricultural detection.
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Anqi Zhao,Mengyun Hu,Zhengying Wu,Yong Wang,Jie Li,Yukou Du
Precisely tuning the morphology of palladium-based alloys is an effective strategy for enhancing the catalytic activity in alcohol electrooxidation. However, methods for synthesizing well-defined nanowires are often not universally applicable and tend to be relatively complex. In this study, we developed a universal method to synthesize PdM nanowires (M = Sn, Pb, Sb, Bi) using a straightforward one-pot solvothermal co-reduction technique. The electronic properties of palladium can be modified through the doping of other elements. The bimetallic synergistic effect endows PdSn nanowires (PdSn NWs) with exceptional catalytic activity in both the ethylene glycol oxidation reaction (EGOR) and the ethanol oxidation reaction (EOR). Specifically, the mass activity of PdSn nanowires in the EGOR was measured at 7.56 A mgPd⁻¹, which is 3.86 times more than that of commercial Pd/C. In the EOR, the mass activity reached 6.43 A mgPd⁻¹, demonstrating an 8.14-fold enhancement over commercial Pd/C. Furthermore, PdSn nanowires also exhibited excellent stability during stability tests. This study provides significant insights into the development of nanowires catalysts with highly efficient alcohol electro-oxidation performance.
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JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Jinjuan Zhao,Sizhuo Ma,Aoxue Zhang,Yuner Xu,Zheng Liu,Mengjie Li,Honglei Yang,Ruifa Jin,Shuwen Li
The hydrogen-bonding interaction among catalytic center, support material and ethanol molecule can establish an effective microenvironment for ethanol oxidation reaction (EOR). However, the surrounding of palladium nanocrystals (Pd NCs) lacks highly electronegative atoms to form hydrogen bonds with ethanol molecule. To effectively address the limitation, suitable molecules can be incorporated into Pd-based catalysts alongside the selection of an appropriate support. The pyrene tetracarboxylate ionic liquid (PTCIL), composed of pyrene tetracarboxylate anions and quaternary ammonium cations, provides abundant oxygen atoms capable of forming hydrogen bonds with ethanol molecules and the oxygen-containing functional groups in reduced graphene oxide (RGO) support, thereby creating a conducive microenvironment towards green EOR. Additionally, PTCIL can be anchored onto the RGO support via π-π stacking, yielding abundant dispersed carboxyl and pyrenyl groups that act as active sites to stabilize Pd NCs. Furthermore, synergistic interactions within the catalyst enable electron transfer from PTCIL to Pd, weakening the adsorption strength of toxic intermediates. Herein, the prepared Pd/PTCIL-RGO-2 exhibits improved electrocatalytic activity (1523.2 mA mg −1 , 5.29 mA cm −2 ) compared to commercial Pd/C (807.2 mA mg −1 , 4.14 mA cm −2 ). This study proposes a design for constructing Pd-based catalysts with tailored local microenvironments, exhibiting enhanced activity and robust durability for versatile applications, including EOR and other small molecule oxidation reactions.
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