ChemCatChem
·
2019
·Vol. 11
·期 20
·5098-5107
·
IF 4.495
Ning Xiang,Yaqin Hou,Xiaojin Han,Yulin Li,Yaoping Guo,Yongjin Liu,Zhanggen Huang
Room temperature HCHO catalytic oxidation over inert support loaded Pd catalysts remains a significant challenge. Herein, a series of alkali Na (1–4 wt.%) modified 1Pd/SBA-15 catalysts were prepared by a co-impregnation method and used for HCHO catalytic oxidation at room temperature. Results showed that alkali Na significantly improved the HCHO oxidation performance of 1Pd/SBA-15 and the optimal Na loading was 2 wt.%. BET, XRD, STEM, XPS, H 2 -TPR, O 2 -TPD and in situ DRIFTS were performed to reveal the promotion role of alkali Na. As a consequence, alkali Na addition could stabilize well dispersed Pd particles which then facilitated the O 2 activation and accelerated the decomposition of formate intermediates species, thus a superior HCHO catalytic oxidation performance was obtained. This study first clearly illustrated the promotion mechanism of alkali Na without the implication of active support and provides an efficient and facile way to achieve high dispersion of Pd particles on inert support and tremendously expands the selected range of supports for room temperature HCHO catalytic oxidation. Graphical Alkali promoted : A series of Na alkali-promoted 1Pd/SBA15 catalysts were prepared by a co-impregnation method and tested for HCHO catalytic oxidation at room temperature. Addition of alkali Na stabilized well-dispersed Pd particles which facilitated O 2 activation and accelerated formate species decomposition rate, leading to superior HCHO catalytic oxidation performance of 2Na-1Pd/SBA-15.
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JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 6
·2302-2314
·
IF 3.5
Dou Yun-Qi,Zhang Qi,Deng Tian-Song,Cheng Zhiqun,Zhao Xiaoyu
Multimetallic plasmonic nanostructures, with appropriate morphology, elemental proportions and sizes, can be used to accelerate photocatalytic reactions. Here, we designed zigzag trimetallic nanostructures with the Au core and Pd–Pt alloy shell, whose catalytic ability was boosted by the synergistic effect of the plasmonic metal and catalytic metal. The catalytic rate of Au@PdPt nanoparticle (NP) with no light have a significant improvement, attributed to the larger contact area provided by the zigzag alloy shell. Furthermore, the enhanced catalytic activity in the presence of light is primarily due to the thermo-photo catalytic effect of plasmonic Au. The adding ratios of Pd:Pt were adjusted from 1:4 to 4:1, and we found that, when adding the Pd:Pt of 1:1, the zigzag Au@PdPt nanoparticle (NP) exhibited a superior reaction rate in the reduction methylene blue (MB) under light illumination. The rate is 8 times higher than that of Au@Pt, and the reduction conversion reached 100%. And it has a favorable plasmon enhancement factor with an appropriate shell thickness and get the balance between the catalytic performance and economic effects. This structure driven by capability-oriented design principles and holds the potential for applications in the field of catalysis. Graphical abstract
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CHEMPHYSCHEM
·
2015
·Vol. 16
·期 18
·3865-3870
·
IF 3.419
Baohua Zhang,Yiguo Xue,Zhimin Xue,Zhonghao Li,Jingcheng Hao
The ionic liquid 1-ethyl-3-methylimidazolium acetate ([EMIM]Ac) is investigated as a solvent for the synthesis of Pd particles. Interestingly, nanosheet-constructed Pd particles could be successfully synthesized in [EMIM]Ac without any additional reducing agent and template under ionothermal conditions. [EMIM]Ac itself works as the solvent, the reducing agent, and the template for the formation of these interesting Pd particles, making this method complementary to the well-known ionic-liquid-precursor approach. Furthermore, [EMIM]Ac can be recycled with no loss of activity for the formation of nanosheet-constructed Pd particles within our studied cycles. Specifically, the nanosheet-constructed Pd particles exhibit superior electrocatalytic activity and stability towards ethanol oxidation and formic acid oxidation compared with commercially available Pd black catalyst, thus demonstrating their promising applications in fuel-cell area. The current approach, thus, presents a green approach towards the synthesis of Pd particles, using only a simple palladium salt and an ionic liquid. Graphical A neat synthesis : A facile green route is proposed for the synthesis of nanosheet-constructed Pd particles in an ionic-liquid solvent without any additional reducing agent and template for efficient electrocatalytic applications.
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Science China-Materials
·
2018
·Vol. 62
·期 3
·351-358
·
IF 4.318
Tang Yonghua,Zhou Peng,Chao Yuguang,Lin Fei,Lai Jianping,Li Hongxing,Guo Shaojun
Photocatalytic hydrogen production represents a promising strategy for clean, sustainable, and environmentfriendly energy supply. Up to now, great efforts have been devoted to designing the photocatalysts with noble metal as co-catalyst for visible-light-driven hydrogen evolution, while more efficient photocatalytic systems are still a major challenge. Herein, we report a facile strategy for synthesizing face-to-face ultrathin Pd nanosheets-amorphous carbon nitride (Pd NSs-ACN) structure with large contacting interface and short electronic transmission pathway, which can work as an efficient photocatalyst for hydrogen production. The synthesis starts with the growth of ultrathin Pd NSs, followed by assembly with the visible-light-response ACN through a simple stirring and annealing procedure. The resultant two dimensional face-to-face structures deliver an average hydrogen generation rate of 1.45 mmol h −1 g −1 at a temperature of 25°C, almost 2.6 times higher than that of Pd Nps-ACN with particle- to-face structural feature. The efficient photocatalytic activity is ascribed to the formation of high-density of active sites between ultrafine face-to-face contacted Pd NSs and the ACN, which cooperate more synergistically towards photocatalytic hydrogen production. The face-to-face engineered Pd NSs-ACN hybrids also offer a good stability revealed by photocatalytic hydrogen production measurements. The extraordinary performance highlights a powerful engineering model for designing other face-to-face contacting co-catalyst/photocatalysts, which will be a great impetus to optimize new catalytic transformations.
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NANOTECHNOLOGY
·
2020
·Vol. 31
·期 13
·135703
·
IF 3.551
Ruiwen Yan,Xiaoyu Sun,Xiaoling Zhang,Jun Zheng,Baokang Jin
In the present work, Pd–Pt nanoparticle/polyaniline/carbon nanotube (NP/PANI/CNT) composites, synthesized through the uniform distribution of Pd–Pt NPs, whose single size was controlled to 2–4 nm by citric acid, on a PANI/CNT compound, served as the electrode catalysts for effective methanol oxidation. The structural characteristics were identified by x-ray diffraction, x-ray photoelectron spectroscopy, scanning electron microscopy, and transmission electron microscopy, and revealed that the Pt65Pd35 NP/PANI/CNT composite displayed superior electrocatalytic oxidation performance and vitality in various Pd–Pt NPs. The results indicated that as an excellent anode catalyst the complex would have application prospects for effective methanol oxidation.
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CATALYSIS LETTERS
·
2026
·Vol. 156
·期 9
·242
·
IF 2.5
Shi Guopu,Shi Fangxu,Liang Fuxin,Wei Yulin,Li Yuanguang,Han Yubing,Wu Junyan,Huang Sai,Wang Honglei,Ji Jun,Wu Chao
Ethyl 3-piperidine-carboxylate is an important intermediate in the pharmaceutical field. To break through the limitations of poor mechanical strength and thermal stability of catalysts and low catalytic efficiency of foam ceramic carriers due to the lack of active sites in traditional synthesis, this study used the hydrogenation synthesis of ethyl nicotinate to produce this intermediate as the probe reaction. Pd-Ni/Ru-Al 2 O 3 -SiO 2 foam ceramic catalysts were prepared by the sol-gel method and the impregnation method. Relying on the bimetallic differentiated synergistic effect of Ni, Ru, and Pd, the above technical bottlenecks were overcome. A variety of characterization techniques reveal its core mechanism of action: Pd serves as the catalytic core, and Ni can optimize the electronic structure, enabling the Pd-Ni alloy to obtain the optimal d-band center and adsorption energy, laying an electronic foundation for efficient catalysis. Ru can precisely control the particle size of Pd-Ru alloy, which is 4.5 nm smaller than that of single-metal Pd, significantly improving the metal dispersion and the utilization rate of active sites. The three-dimensional network structure of foam ceramics enhances mass transfer efficiency. The γ-Al 2 O 3 -SiO 2 coating provides abundant active sites and excellent stability. The catalytic performance of this system has been significantly enhanced. Among them, the yield of the corresponding product of the Pd-Ni bimetallic catalyst reached 92.57%, and it still remained above 80% after five cycles of use, providing new prospects for the green and efficient synthesis of ethyl 3-piperidine-carboxylic acid esters and the development of low-cost hydrogenation catalysts. Graphical
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Jing Li,Sizhuo Ma,Dingyuan Yi,Ruonan Liu,Pengxue Li,Yanjun Cui,Jia Wei,Shuwen Li
The combination of electronic state engineering and surface-clean control represents a viable strategy for developing advanced electrocatalysts toward the ethanol oxidation reaction (EOR). Herein, the phosphorus-containing functional groups (oxidized P species) modified reduced graphene oxide (PG) with three dimensional (3D) hierarchical macrostructures was synthesized by a common hydrothermal method, and ultrafine surface-clean Pd NCs were equably anchored on PG through a facile hydrogen balloon reduction strategy in the absence of surfactants or organic solvents (Pd/PG). In the alkaline EOR, Pd/PG delivers significantly enhanced catalytic activity (with a mass activity of 2302.0 mA mg −1 ) alongside remarkable long-term operational durability and stability, distinctly surpassing both Pd/G and commercial Pd/C. Combined characterization and experimental study attest the enhanced electrocatalytic behavior of Pd/PG is derived from the linkage of oxidized P species and surface-clean control. Surface-clean Pd NCs and 3D hierarchical macrostructures affords a free exchange of reactants/products and dramatically facilitate mass/electron transfer during EOR. The linkage of oxidized P species makes electron transfer from PG to Pd and generates an increased electron density at Pd sites, leading to a reduced energy barrier for CO ads oxidation and enhanced OH ads adsorption, thereby collectively promoting the catalytic activity and long-term operational durability. Meanwhile, interfacial electron transfer fosters a stronger Pd-support interaction, thereby suppressing agglomeration, dissolution, and Ostwald ripening during the EOR process and ultimately bolstering the long-term durability of the catalyst. This study establishes that synergistic surface-clean and interfacial engineering enhances electrocatalysis, informing the development of advanced carbon-supported electrocatalytic materials.
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ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Heyu Wang,Ou Wang,Yu Tang,Wenxiu Xiao,Bao-Li An,Yongmei Zhao,Bo Lu,Xiaohong Wang,Jiaqiang Xu
As an effective sensitizer for chemiresistive hydrogen (H 2 ) sensors, the practical application of Palladium (Pd) is limited by the Sabatier principle, where intrinsically strong Pd─H binding leads to sluggish desorption kinetics and prolonged response and recovery time. A high-entropy alloying strategy was proposed to tailor the local coordination and electronic structure of Pd active sites and weaken the Pd─H binding. Pd x (FeCoNiCu) 1− x ( x = 0.05–0.35)high-entropy alloys (HEAs) were synthesized as sensitizers for SnO 2 to improve its H 2 sensing reactivity, especially its response and recovery rate. Pd 0.2 (FeCoNiCu) 0.8 -SnO 2 sensor exhibits short response and recovery time (0.6 s/2.0 s), a high response of 18.8 toward 100 ppm H 2 (4.06 times higher than Pd-SnO 2 ), a practical detection limit of 1 ppm and a long-term stability (>90% retention over 50 days). The working window of the sensor is also wider, which exhibits a linear response in both low (20–120 ppm) and high (4000–20 000 ppm) H 2 concentration ranges. Experimental analysis and theoretical calculation attribute this performance to the downshift of the Pd d -band center (from −1.84 to −2.57 eV). The electronic modulation alleviates the strong binding of hydrogen intermediates, thus leading to ultrafast response and recovery without compromising sensitivity.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Yimeng Zhou,Tingting Chen,Jie Ding,Hao Li,Di Wu,Xuran Xu,Qin Zhong
Controlled hydrogen spillover is of paramount importance for the precise regulation of target products in the hydrogenation selectivity. In this study, Pd@1Al2O3/Ag catalyst was designed and prepared for the hydrogenation-acetalization of diethyl oxalate (DEO) to 1,1-diethoxyethane (DEE) with excellent DEE selectivity (83.0%) and high DEO conversion (99.9%). Pd species are mainly responsible for the generation of H* species from H2 adsorption and dissociation, and Al2O3 acted as a delivery channel for H* species to migrate and mass transfer from H* to Ag nanoparticles loaded on the catalyst surface, which facilitated the progression of subsequent DEO hydrogenation-acetalization reactions. This study provides a promising strategy for high hydrogenation-acetalization efficiency via controllable hydrogen spillover.
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PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.2
Run Pan,Abubakar Yusuf,Chengjun Wang,Jianrong Li,Zhiyu Xiao,Shuai Liu,Yidong Zhong,Yong Ren,Zheng Wang,Hainam Do,John L. Zhou,George Zheng Chen,Jun He
Natural gas vehicles (NGVs) offer significant environmental advantages by reducing pollutant emissions, but effective exhaust treatment remains a challenge due to high methane emissions and catalyst deactivation over time. This study introduces a core-shell Pd@CeO 2 /Al 2 O 3 three-way catalyst (TWC) designed to enhance the efficiency and durability of NGV exhaust treatment. The core-shell structure significantly improves catalytic performance. The optimized Pd@Ce/Al (S-500) catalyst demonstrates excellent low-temperature activity, with T 50 values of 336 °C for CH 4 and 397 °C for NO. It also achieves remarkable reductions of 113 and 177 °C in the T 90 for CH 4 and NO conversion, respectively, compared to the non-core-shell counterpart, Pd-Ce/Al (S-500). Characterizations reveal enhanced metal-support interactions, increased oxygen vacancies, and optimized Pd-CeO 2 interfaces as key active sites. Density functional theory calculations further demonstrate that the core-shell structure facilitates electron transfer at Pd-CeO 2 interfaces and lowers energy barriers for three-way reactions, enhancing catalytic efficiency. Notably, the core-shell Pd@Ce/Al (S-500) catalyst maintains high conversion efficiency for CH 4 and NO, with only slight losses (5.5% and 6.6%, respectively) over a 100-h time-on-stream stability test, following 16 h of harsh hydrothermal aging at 800 °C, showcasing its long-term stability. These findings provide a deeper understanding of the role of the core-shell Pd@CeO 2 structure in Pd-based TWCs and offer valuable insights for designing durable and efficient catalysts to meet the stringent emission standards of NGVs.
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高影响因子
INTERNATIONAL IMMUNOPHARMACOLOGY
·
2026
·
IF 5.6
Songping Wang,Shuai Zhou,Jiankang Huang,Qing Pang,Hao Jin,Huichun Liu
This study elucidates how H3K4 methylation-driven upregulation of Calbindin 2 (CALB2) promotes immune evasion and chemoradioresistance in cholangiocarcinoma (CCA). Integrated bioinformatics analyses identified CALB2 as a hub gene linked to an immunosuppressive microenvironment. In vitro, CALB2 knockdown suppressed tumor cell proliferation, migration, invasion, and calcium signaling—evidenced by reduced phosphorylation of CaMKII, PKC, and NF-κB—while increasing apoptosis. Mechanistically, CALB2-activated NF-κB transcriptionally upregulated Keratin 7 (KRT7), which subsequently induced PD-L1 expression. This CALB2/KRT7/PD-L1 axis impaired T cell activation, reducing CD69 and IFN-γ expression. In vivo, CALB2 silencing inhibited tumor growth, downregulated PD-L1 and Ki-67, and enhanced apoptosis. Notably, CALB2 knockdown significantly sensitized CCA tumors to gemcitabine plus radiotherapy, an effect attenuated by KRT7 overexpression. These findings define a novel H3K4 methylation/CALB2/calcium/NF-κB/KRT7/PD-L1 signaling axis that drives immune suppression and therapy resistance in CCA, highlighting its potential as a multi-target strategy for combined immunotherapy and chemoradiotherapy.
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PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Qiaozhi Han,Chengxu Li,Yunshu Wang,Ziwei Ma,Chengyu Duan,Yucong Yin,Zichen Bao,Yonghao Shen,Chenwen Yin,Zhuofeng Hu,Qiming Sun
Abstract The direct synthesis of hydrogen peroxide (H2O2) from H2 and O2 provides a sustainable route for decentralized oxidant production, but its practical use is limited by inefficient Pd utilization, undesired H2O2 decomposition, and the need for high noble-metal loadings. Here, we report a Ni(OH)2-promoted Pd@S-1 catalyst that integrates zeolite confinement with interfacial electronic modulation for efficient aqueous H2O2 synthesis. The optimized Pd4Ni1@S-1-H catalyst delivers an H2O2 productivity of 3.39 mol gPd–1 h–1 under acidic conditions, representing the highest value among reported semibatch glass reactor systems and a 10-fold improvement in Pd utilization efficiency relative to a commercial Pd/C catalyst. Advanced spectroscopic analysis and density functional theory calculations reveal that Ni(OH)2 donates electrons to Pd, lowering the average Pd valence state from 1.83 to 1.39, and serves as a hydrogen-transfer bridge that promotes hydrogen migration to the *O–O intermediate. Meanwhile, hydrophobic silicalite-1 (S-1) zeolite micropores enrich dissolved H2/O2 and suppress secondary H2O2 decomposition by facilitating product desorption. The resulting in situ H2O2 generation system enables efficient Cr(VI) reduction, highlighting its potential for sustainable water remediation.
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