Surfaces and Interfaces
·
2025
·
IF 6.3
Rui Xu,Jingqi Bao,Ningru Xuan,Bingxin Zhou,Lingshan Liao,Qiusheng Zhou,Di Wu,Linfang Lu
The template sacrifice method is a pivotal strategy for synthesizing noble metal-based nanocrystals with enhanced catalytic properties. A critical limitation of this method lies in the challenges associated with regulating the morphology of the resultant nanocrystals. This study demonstrates that the morphology of PtCu nanocrystals can be effectively modulated by adjusting the pH in the Cu 2 O template sacrifice method. Various PtCu nanocrystals, including PtCu hollow nanoboxes and PtCu nanodendrites of differing sizes, have been successfully synthesized. Mechanistic investigations reveal that reduced pH corresponds to a lower electrode potential of Cu 2 O, which enhances its reducing capacity, thereby intensifying the galvanic replacement reaction with the Pt precursor. The driving force of Kirkendall effect during this process can be systematically manipulated via pH adjustments, leading to the generation of PtCu nanocrystals with diverse morphologies. The synthesized PtCu nanocrystals demonstrate significantly improved methanol oxidation reaction activity compared to commercial Pt/C. Specifically, the PtCu hollow nanoboxes exhibit a methanol oxidation reaction (MOR) activity of 1.93 A mg⁻¹, which is 5.4 times greater than that of the commercial Pt/C. Physical characterizations suggest that the superior catalytic performance of PtCu hollow nanoboxes catalyst is attributed to its increased surface electronic density of Pt resulting from the special hollow and porous morphology. The pH control strategy outlined in this research holds promise for the synthesis of other Cu-based nanoalloys with varying morphologies, and may be applicable to other catalytic systems.
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FUEL
·
2025
·
IF 7.5
Xiang Tan,Peng Luo,Liya Cao
Hydrodeoxygenation (HDO) is pivotal for upgrading lignin-derived streams into drop-in aviation fuels. Efficient aryl C–O bond cleavage with complete deoxygenation typically requires harsh conditions. Here we report electron-rich Pt nanocatalysts that convert lignin-derived model compounds and lignin oil to jet-range cycloalkanes under notably mild conditions (100 °C, 10 % H 2 /Ar at 0.5 MPa). Alkyl cyclohexanes are obtained in 95.2 % yield from a representative model substrate and 90.5 % from lignin oil. Time-resolved profiling and cascade-kinetics analysis indicate that aryl C–O bond scission is the rate‑determining step. Differential charge density and reaction free‑energy analyses support that increasing electron density on Pt promotes H* activation and lowers the free‑energy change (ΔG) for C–O cleavage, consistent with the enhanced activity. The catalysts exhibit broad substrate scope and reusability. This work provides a practical low-temperature route and an electronic-structure design principle for energy-efficient upgrading of lignin-derived oils to jet-range cycloalkanes.
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Catalysts
·
2025
·Vol. 15
·期 11
·
IF 4
Juan Du,Wanting Qiu,Sunbal Ayaz,Jian Long,Wenze Guo,Ling Zhao,Zhenhao Xi
2,5-furandicarboxylic acid (FDCA), a high-value biomass-derived monomer, serves as a crucial building block for sustainable polymers including polyesters, polyamides, and polyurethanes. This study systematically investigated the catalytic oxidation of 5-hydroxymethylfurfural (HMF) to FDCA over Pt/Al2O3and Pt–Bi/Al2O3catalysts. The 5Pt/Al2O3catalyst yielded 60.6% FDCA after 12 h under optimized conditions (80 °C, 0.1 MPa O2, 1 equiv. Na2CO3). Remarkably, Bi-modified 5Pt–1Bi/Al2O3catalyst dramatically enhanced catalytic performance, achieving 94.1% FDCA yield within 6 h under optimized conditions (80 °C, 1.5 MPa O2, 2 equiv. Na2CO3). Comprehensive characterization revealed that the exceptional activity originates from Bi–O–Pt interactions that modulate the electronic structure and oxidation state of Pt active sites, which facilitates the oxidation of intermediate 5-formyl-2-furancarboxylic acid (FFCA) to FDCA, the rate-limiting step of HMF oxidation. This work demonstrates an efficient Bi-promoted Pt catalytic system for FDCA production with significant potential for industrial application.
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Nature Communications
·
2025
·Vol. 17
·期 1
·90
·
IF 15.7
Tuo Yongxiao,Qu Jingying,Sun Huailu,Lu Qing,Wang Bin,Gai Hongwei,Yin Defu,Feng Xiang,Chen De
Catalyst design is often reaction-specific due to the lack of universal descriptors linking molecular structures to optimal active-site configurations. Here, we uncover a reactant-dependent volcano relationship in Pt-catalyzed dehydrogenation, governed by the Pt-Pt coordination number (CN Pt-Pt ). Using a tunable Pt/MgAl 2 O 4 system, we identify optimal CN Pt-Pt values of ~2.5, ~4.7, and ~7.0 for cyclohexane, methylcyclohexane, and decalin, respectively. This activity trend is explained by an orbital hybridization-guided mechanism, where optimal activity emerges from a balance between C-H bond activation and product desorption, mediated by the interactions between Pt d-orbitals and the π* orbitals of dehydrogenated intermediates. We introduce the LUMO energy of aromatic products as a universal electronic descriptor that serves as a proxy for π* orbital energy. LUMO energy shows strong linear correlations with the d-band center of Pt at the optimal CN Pt-Pt , enabling rational tuning of electronic interactions across diverse reactants. The optimized Pt/MgAl 2 O 4 catalyst delivers 2-3 times higher activity with >100 h stability under industrial conditions at only 300 o C, offering a robust strategy for hydrogen release and active-site engineering in dehydrogenation catalysis.
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PubMed
高影响因子
Catalysts
·
2025
·Vol. 15
·期 3
·220
·
IF 4
Jiani Chen,Yanxuan Wang,Jianghua Huang,Shuting Ma,Yiyang Zhang,Fukun Bi,Xiaodong Zhang
Nowadays, volatile organic compounds (VOCs) increasingly jeopardize ecosystem sustainability and human well-being. In this study, UiO-66 and its different electron beam (EB) irradiation doses (100, 300, 500 kGy) modified materials supported Pt catalysts, Pt/UiO-66 and Pt/UiO-66-X (X = 100, 300, and 500, representing the irradiation doses), were synthesized, and a series of characterizations were conducted on the samples. On this basis, the effectiveness of these catalysts was evaluated through the degradation of ethyl acetate. The study findings indicated that the sample irradiated at 100 kGy demonstrated superior catalytic performance. Thereafter, extensive tests with regard to water resistance, stability, and cycle performance indicated that the Pt/UiO-66-100 catalyst was characterized by satisfactory reusability and catalytic stability, even when faced with high heat and humidity. Further work with in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and thermal desorption–gas chromatography–mass spectrometry (TD-GC–MS) uncovered the process of degradation of ethyl acetate. This research provides a guideline for the design of high-performance VOC degradation catalysts through EB modification.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Lingya Yi,Yang Yu,Yuzhou Tao,Weihua Hu
Pt-based intermetallic nanoparticles demonstrate impressive oxygen reduction reaction (ORR) activity and durability due to their atomically ordered nature but their synthesis remains a tremendous challenge. Herein we report Pt–Co intermetallic nanoparticles anchored on nitrogen-rich graphene (NG) nanosheets for efficient ORR electrocatalysis in acidic media. The rich nitrogen atoms, doped via low-temperature plasma treatment on graphene efficiently inhibit the sintering of the nanoparticles during high temperature annealing via strong metal-support interaction and enhance the anchoring stability. Meanwhile, the electronic interaction between NG and Pt–Co intermetallic nanoparticles negatively shifts the d-band center of Pt to enhance their intrinsic ORR activity. As-prepared PtCo/NG-900 with low Pt loading of 3.4 μg cm −2 exhibits high mass activity of 1.28 A mg −1 at 0.8 V vs. RHE, and enhanced durability with only 1.9 mV decay in half-wave potential (E 1/2 ) after 2000 potential cycles.
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Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 41
·35690-35700
·
IF 9.5
Quanming Ren,Xiaoya Zhao,Liping Zhou,Linghe Song,Juntai Tian,Jisheng Nie,Peng Liu,Daiqi Ye,Zhi Wang
Metal–support interaction (MSI) plays an essential role in affecting the catalytic activity of supported catalysts by establishing a unique interface between metal and the support. However, moderate modulation of MSI remains a major challenge, as both too weak and extremely strong MSI can lead to catalysts exhibiting inferior catalytic activity. Herein, a series of Pt catalysts supported on ceria with various levels of sodium modification were prepared via a facile impregnation method. A comprehensive investigation based on experimental studies and Density Functional Theory (DFT) calculations substantiates that the addition of sodium, as an effective motivator, triggers more significant electron transfer from Pt clusters to the CeO2 support accompanied by the formation of an interfacial sites (Ptδ+–OV–Ce3+), indirectly involved in reactions to decrease the activation energy of lattice oxygen in Pt–O–Ce, and Pt/1.1Na–CeO2 with moderate MSI is conducive to the oxygen species on the CeO2 adjacent to the Ptδ+ (e.g. Ptδ+–OV–Ce3+) configuration at the interface to take part in toluene oxidation. And the perimeter Pt0–OV–Ce3+ sites, as the active site, were formed by the Pt nanoparticles on the CeO2 for toluene adsorption. Pt/1.1Na–CeO2 (1.57 nm) with small particle size possesses a much larger number of perimeter Pt0–OV–Ce3+ sites than Pt/CeO2. Therefore, the catalytic activity and stability of Pt/1.1Na–CeO2 were remarkably enhanced in toluene oxidation compared to those of Pt/CeO2. This work emphasizes that alkali can be employed as a motivator to regulate MSI, providing a facile and powerful approach to design efficient catalysts for VOC oxidation.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Xuan-Yu Yang,He-Jie Wang,Hao-Nan Chen,Li-Juan Yue,Fei-Long Gong,Ke-Feng Xie,Shi-Zhong Wei,Yong-Hui Zhang
Electronic modulation of Pt sites is of great significance in catalytic reaction involved chemical engineering process. Alkali metal doping is a promising strategy to modify the d orbit of Pt, which can effectively affect the reaction between material and adsorbates, however, the relationship is still unclear. Here, we have rationally designed Pt-modified Na-doped WO 3 nanorods, and the electronic modulation of Pt can be finely modified by Na doping. The Pt-Na/WO 3 -Ar nanorods exhibit excellent H₂S sensing performance, with high response (R a /R g = 701 @ 1 ppm), low operating temperature (110 °C), and detection limit as low as 2.42 ppb. Experimental and theoretical results indicate that the introducing of Na effectively enhances the interaction between Pt nanoparticles (NPs) and WO 3 . Additionally, Na doping successfully modulate the d-band center of Pt, optimizing the adsorption and desorption processes during sensing. The synergistic effects of these components enable the Pt-Na/WO 3 -Ar sensor to exhibit outstanding H₂S sensing performance. Notably, the fabricated sensors are further used to monitor the hydrogen sulfide (H 2 S) of halitosis biomarkers, which holds significant application potential in environmental protection and medical diagnostics.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Xue Li,Yan-Rong Liu,Wen-Min Liao,Ai-Ping Jia,Yue-Juan Wang,Ji-Qing Lu,Meng-Fei Luo
Catalytic propane combustion was performed on a series of supported Pt/AlF 3 catalysts. These catalysts are very active and stable in the reaction, and the 0.2Pt/AlF 3 catalyst gives the highest specific reaction rate of 207.3 μmol g Pt −1 s −1 at 220 °C. The 1Pt/AlF 3 is much more active than the reference Pt/Al 2 O 3 catalyst, due to its higher content of metallic Pt species than that in the Pt/Al 2 O 3 . Furthermore, turnover frequency (TOF) based on Pt dispersion increases with the surface concentration of metallic Pt 0 in the catalyst, suggesting these species might be the active sites. Furthermore, synergistic roles of metallic and oxidized Pt species are found, as the TOFs calculated based on surface Pt 0 concentration reaches a maximum at the Pt 0 /Pt 2+ molar ratio of about 1. Such optimal Pt 0 /Pt 2+ ratio implies the requirement of Pt 0 Pt 2+ pair in the reaction, probably due to the activation and cleavage of C H bond on metallic Pt atom and the sequential oxidation on the oxidized Pt atoms.
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CHINESE JOURNAL OF CATALYSIS
·
2017
·
IF 2.813
Honggen Peng,Jiawei Ying,Jingyan Zhang,Xianhua Zhang,Cheng Peng,Cheng Rao,Wenming Liu,Ning Zhang,Xiang Wang
Catalytic oxidation of formaldehyde (HCHO) is the most efficient way to purify indoor air of HCHO pollutant. This work investigated rare earth La-doped Pt/TiO 2 for low concentration HCHO oxidation at room temperature . La-doped Pt/TiO 2 had a dramatically promoted catalytic performance for HCHO oxidation. The reasons for the La promotion effect were investigated by N 2 adsorption, X-ray diffraction, CO chemisorption , X-ray photoelectron spectroscopy, transmission electron microscopy (TEM) and high-angle annular dark field scanning TEM . The Pt nanoparticle size was reduced to 1.7 nm from 2.2 nm after modification by La, which led to higher Pt dispersion, more exposed active sites and enhanced metal-support interaction. Thus a superior activity for indoor low concentration HCHO oxidation was obtained. Moreover, the La-doped TiO 2 can be wash-coated on a cordierite monolith so that very low amounts of Pt (0.01 wt%) can be used. The catalyst was evaluated in a simulated indoor HCHO elimination environment and displayed high purifying efficiency and stability. It can be potentially used as a commercial catalyst for indoor HCHO elimination.
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ADVANCED FUNCTIONAL MATERIALS
·
2017
·Vol. 27
·期 23
·1700359
·
IF 12.124
Yafei Cheng,Shunkai Lu,Fan Liao,Liangbin Liu,Yanqing Li,Mingwang Shao
High overpotentials and low efficiency are two main factors that restrict the practical application for MoS 2 , the most promising candidate for hydrogen evolution catalysis. Here, Rh MoS 2 nanocomposites, the addition of a small amount of Rh (5.2 wt%), exhibit the superior electrochemical hydrogen evolution performance with low overpotentials, small Tafel slope (24 mV dec −1 ), and long term of stability. Experimental results reveal that 5.2 wt% Rh MoS 2 nanocomposite, even exceeding the commercial 20 wt% Pt/C when the potential is less than −0.18 V, exhibits an excellent mass activity of 13.87 A mg metal −1 at −0.25 V, four times as large as that of the commercial 20 wt% Pt/C catalyst. The hydrogen yield of 5.2 wt% Rh MoS 2 nanocomposite is 26.3% larger than that of the commercial 20 wt% Pt/C at the potential of −0.25 V. The dramatically improved electrocatalytic performance of Rh MoS 2 nanocomposites may be attributed to the hydrogen spillover from Rh to MoS 2 .
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NANO
·
2013
·
IF 1.167
SHIYONG BAO,HAN ZHU,PAN WANG,MEILING ZOU,MINGLIANG DU,MING ZHANG
A facile and green route was introduced to synthesize Pt nanoparticles (PtNPs) immobilized on Cu 2 O octahedrons to form Cu 2 O – Pt hierarchical heterostructure. Transmission electron microscopy (TEM), field emission scanning electron microscopy (FE-SEM), high resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) were employed to study their morphology, chemical and crystallographic properties of the Cu 2 O – Pt hierarchical heterostructure. These novel Cu 2 O – Pt hierarchical heterostructures show fascinating degradations of methylene blue (MB), due to the suppressed electron/hole recombination phenomena and the efficient ability to capture the light.
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