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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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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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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
·
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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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
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2024
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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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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
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IF 3.8
Xuhai Zhu,Xiaobing Li,Rongjun Lin,Rui Lu,Fang Lu
Designing efficient catalysts for the preferential hydrogenation of vinyl groups is a pivotal challenge in the production of pharmaceuticals, agrochemicals, fine chemicals, dyes, and other valuable compounds. Herein, we developed evenly dispersed bimetallic Pd–Co nanoparticles on mesoporous silica nanospheres (MSNs) for selective hydrogenation of a model compound 3-nitrostyrene. By tuning the Pd/Co molar ratio and solvents, the efficiency of 3-nitrostyrene hydrogenation to 3-ethylnitrobenzene with the Pd1–Co1/MSN-Nb catalyst was well optimized; while 3-nitrostyrene was converted entirely, the selectivity of 3-ethylnitrobenzene was up to 95%. Moreover, this catalyst was stable and compatible with styrene and its derivatives. Further characterization results indicated that the combined effect of Pd-based metal nanoparticles and MSN-Nb and the electronic interaction between Pd and Co components in the Pd1–Co1/MSN-Nb catalyst have significant importance in the hydrogenation of 3-nitrostyrene. The aforementioned catalytic system will prove invaluable in guiding the selective hydrogenation of vinyl groups.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
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IF 19
Leilei Yin,Yuyan Liu,Shuai Zhang,Jin-Cheng Liu,Yong Jiang,Yaping Du
Excessive adsorption of oxygen-containing intermediates during oxygen reduction reactions (ORR) on palladium (Pd)-based materials is a critical factor limiting their catalytic activity. Alloying presents a powerful strategy to overcome this inherent challenge. In this study, the alloying of the low electronegativity lanthanide gadolinium (Gd) with Pd is explored. Pioneering theoretical calculations indicate that Gd, acting as an electron donor, induces charge redistribution between the metals. This process weakens the over-adsorption of OH* intermediates on the Pd surface and reduces the reaction overpotential. Subsequent experiments yield Pd 3 Gd solid-solution nano-alloys supported on conductive carbon black (Pd 3 Gd/C-600), resulting in a 30 mV enhancement in half-wave potential and a 4.5 fold increase in mass activity in an alkaline medium compared to Pd/C-600. Due to its superior performance in ORR, Zn-air batteries utilizing Pd 3 Gd/C-600 cathodes demonstrate remarkable peak power density and stability over 330 h. This study offers valuable insights into the rational design of rare earth alloys and their catalytic chemistry in ORR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yanwei Sun,Guangyan Xu,Chang Liu,Yajie Pan,Yingjie Wang,Yunbo Yu,Hong He
Although palladium-based catalysts exhibit excellent methane oxidation activity, sulfur poisoning still leads to severe deactivation. To overcome this, we synthesized an oxide-zeolite (OXZEO) composite, Ce x /Pd@MFI, via combined hydrothermal treatment and ball milling . In the resulting architecture, PdO x active sites are spatially confined within the MFI framework, while CeO 2 nanoparticles uniformly decorate the external surface as protective species. The optimized Ce 3 /Pd@MFI catalyst demonstrated markedly enhanced sulfur resistance, achieving a T 50 —the temperature at which 50 % CH 4 conversion occurred—of 361 °C after sulfation with 100 ppm SO 2 . Moreover, Ce 3 /Pd@MFI maintained sulfur-resistant stability for 110 h, far surpassing Pd@MFI and Pd/Al 2 O 3 , which rapidly deactivated upon exposure to SO 2 for bare 1 h. Furthermore, we proposed a redox-atmosphere switching method to regenerate sulfated CeO 2 protective species, thereby enabling the Ce x /Pd@MFI catalysts to maintain durable sulfur tolerance. The broad applicability of the OXZEO design was further confirmed in CO oxidation : Ce 3 /Pd@MFI remained stable under high SO 2 concentrations during CO oxidation. This work establishes a paradigm for engineering sulfur-resistant palladium catalysts via synergistic spatial confinement and protective-site incorporation, offering critical insights for the development of robust emission-control catalysts in sulfur-rich environments.
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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.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Danhong Gao,Shasha Gao,Hanling Deng,Hongwei Liu,Dusong Hou,Qianyao Lu,Xinjian He,Sheng Huang
Modulating the surface electronic structure of metal oxides is crucial for enhancing their gas-sensing performance, with gradient energy level structures offering effective regulate. However, the mechanism underlying their impact on hydrogen sensing remains unclear. This study constructed mesoporous Pd-PdO/SnO 2 double-shelled microspheres with gradient energy levels via a soft-template method, precisely tuning the surface electronic structure of SnO 2 . The architecture integrates high surface area (30.9 m 2 /g), ordered mesopores (17.9 nm), and Schottky barrier modulation at PdO(5.04 eV)-SnO 2 (4.92 eV) interfaces, establishing unidirectional electron transfer pathways that amplify charge separation efficiency by 7.3×. The optimized 5 at.% Pd-PdO/SnO 2 sensor achieves high H 2 response (R a /R g = [email protected] ppm) at 162.5℃ with ultrafast kinetics (0.2 s response/4.8 s recovery), a three-order detection span (0.5–8000 ppm), and humidity tolerance (91 % accuracy@80 %RH via machine learning). Theory calculation reveals the gradient structure enhances H 2 adsorption energy (−0.76 eV vs. PdO/SnO 2 : −0.02 eV) and boosts interfacial charge transfer by 46× (0.276 e vs. 0.006 e), driven by synergistic mechanisms: (1) Sn 5 s/p-dominated conduction band electron enrichment (68 % DOS increase near Fermi level), and (2) Pd catalytic activation lowering H 2 dissociation barriers from 1.32 eV (SnO 2 ) to 0.85 eV. This electronic-structure engineering paradigm establishes a roadmap for intelligent gas sensors.
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DIAMOND AND RELATED MATERIALS
·
2025
·
IF 5.1
Ruixi Li,Jiani He,Huan Fu,Qingqing Liu,Lihua Zhu,Weizhen Wang,Liqing Li,Zhiqing Yang,Huan Zhang,Hengqiang Ye
Graphitic carbon nitride (g-C 3 N 4 ) is prepared by high-temperature annealing method, followed by the deposition of noble metal (Pt, Rh, Pd, Ru) nanoparticles and then variants 0.38 wt%, 0.76 wt%, 2.51 wt%Pd/g-C 3 N 4 catalysts are obtained using NaBH 4 reduction method. Pd/g-C 3 N 4 exhibits excellent catalytic activity in nitroarenes selective hydrogenation under quite moderate reaction conditions (e.g., p-nitroacetophenone hydrogenation, 96.5 % conversion with 100 % selectivity to p-aminoacetophenone and 15.6 min −1 -turnover frequency at 3.0 MPa H 2 , 20 °C, 0.33 h). Additionally, the Pd/g-C 3 N 4 samples are used for 1, 3-dinitrobenzene hydrogenation, 2.51 wt%Pd/g-C 3 N 4 obtains 97.6 % conversion and 100 % selectivity to m-nitroaniline (20 °C, 3.0 MPa H 2 , 1 min). TOF: 2.51 wt%Pd/g-C 3 N 4 -2.02 s −1 > 0.76 wt%Pd/g-C 3 N 4 -0.56 s −1 > 0.38 wt%Pd/g-C 3 N 4 -0.54 s −1 for 1, 3-dinitrobenzene hydrogenation. Characterizations of XRD, XPS, AC-STEM, AC-STEM elemental analysis, TEM, HRTEM, BET and H 2 -TPD, etc. demonstrate that the Pd nanoparticles in Pd/g-C 3 N 4 have high dispersion and surface/interface synergy of Pd-g-C 3 N 4 , probably contributing to the catalyst's enhanced selectivity, activity, and stability in nitroaromatics hydrogenation. In addition, the catalyst is recyclable and highly durable for nitroaromatics hydrogenation.
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