ChemistrySelect
·
2024
·Vol. 9
·期 1
·e202303384
·
IF 1.9
Shiqin Lai,Zhibing Kang,Lie-Yuan Zhang,Dengke Wang,Lanqing Deng,Jian-Ping Zou
Graphical Ultrafine Pd nanoparticles (1.41 nm)-embedded MIL-100(Fe) (Pd-MOF-Fe) nanocomposites are synthesized via a double-solvent impregnation integrated with photo-reduction approach. Coupling MOF-based catalysis with Pd-based catalysis, the resultant Pd-MOF-Fe shows excellent catalytic efficiency and high stability toward visible-light-induced dehydrogenation of alcohols to hydrogen evolution and value-added carbonyl chemical production. Solar-driven hydrogen (H 2 ) evolution combined with synchronously selective oxidation for fine chemicals production is of great significance in energy and synthetic chemistry. Herein, ultrafine Pd nanoparticles-encapsulated MIL-100(Fe) (Pd-MOF-Fe) nanocomposites are synthesized through double-solvent impregnation integrated with photo-reduction method. Integrating MOF-based catalysis and Pd-based catalysis, the Pd-MOF-Fe can serve as multifunctional catalyst for photoinduced alcohol dehydrogenation reaction. Optimal generation rates of H 2 (3.61 mmol g −1 h −1 ) and benzaldehyde (3.40 mmol g −1 h −1 ) are gained over Pd-MOF-Fe, ca. 4.1 times that of the Pd/MOF-Fe, in which Pd crystals with size ranging from 3 to 6 nm are immobilized on the intersurface of MOFs. Besides, controlled experiments reveal the pivotal role of the opened FeO 6 nodes of MIL-100(Fe) as Lewis acid sites toward alcohol activation. This work provides a controllable approach for metal nanoparticle immobilization. Furthermore, considering the diversified MOF structures, this study also highlights the infinite possibility of metal nanoparticle/MOFs as multifunctional platform for solar energy conversion and chemicals production.
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高影响因子
RARE METALS
·
2024
·
IF 9.6
Hu Xiao-Jie,Sun Yu-Han,Liu Ling-Yue,Mao Dan-Jun,Zheng Shou-Rong
Monochloroacetic acid (MCAA) is identified as a highly carcinogenic disinfection by-product in chlorinated drinking water. In this study, a series of CeO 2 -supported Pd catalysts (Pd/MCeO 2 ) were synthesized through one-step calcination of Pd-loaded Ce-UiO-66-BDC (Ce-MOF), and the liquid-phase catalytic hydrodechlorination of MCAA was explored using these catalysts. For comparison, Pd/CeO 2 catalysts were additionally synthesized using the conventional impregnation method. The characterization results reveal that the catalysts exhibit strong metal–support interaction, leading to high Pd dispersion and Pd n + content. Additionally, the calcination temperature significantly influences catalytic performance, with the catalyst calcined at 500 °C (Pd/MCeO 2 -500) demonstrating the highest catalytic activity and achieving complete dechlorination of MCAA within 50 min. Furthermore, it is found that the catalytic MCAA hydrodechlorination using the catalysts adheres to the Langmuir–Hinshelwood model. Accordingly, low reaction pH is favorable for the catalytic hydrodechlorination of MCAA, enhancing MCAA adsorption on the catalyst surface due to the electrostatic interaction between MCAA and the catalyst surface. Theoretical results suggest that the presence of Pd n + efficiently facilitates MCAA adsorption and C–Cl cleavage, thus significantly enhancing the liquid-phase catalytic hydrodechlorination. Graphical abstract
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高影响因子
LANGMUIR
·
2026
·
IF 3.9
Jingyun Zhao,Qian Lin,Yongyong Shi,Keliang Wang,Hongyan Pan
The direct synthesis of H2O2 from H2 and O2 is a sustainable alternative to the anthraquinone process, but its selectivity is severely limited by competing side reactions together with H2O2 hydrogenation and decomposition, while catalyst degradation and Pd leaching during operation further aggravate the loss of selectivity. In this study, we address these challenges by developing KBr-modified hollow core–shell Pd catalysts. The catalysts were synthesized with controlled KBr incorporation and subjected to thermal treatment to stabilize their electronic structure. Comparative catalytic tests, combined with electron microscopy, X-ray photoelectron spectroscopy, temperature-programmed reduction, and elemental analysis, revealed that KBr modification combined with thermal treatment helps maintain the stability of Pd2+ species, preventing their reduction during catalyst preparation and reaction, while also suppressing Pd leaching. Meanwhile, the hollow core–shell architecture physically confines Pd nanoparticles and minimizes detachment. As a result, the modified catalysts exhibited significantly improved selectivity and long-term cycling stability. These findings demonstrate that halide modification enhances catalyst performance not through simple site poisoning but via electronic modulation and structural stabilization, providing a new strategy for designing selective and durable catalysts for direct H2O2 synthesis.
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PubMed
高影响因子
CATALYSIS LETTERS
·
2026
·Vol. 156
·期 7
·191
·
IF 2.5
Liu Yubing,Tang Jie,Cai Chenyu,Gu Runjing,Yang Xinyu,Yue Liang,Bai Yiqiang,Zhang Fengxiao,Liang Jing,Xu Naizhang,Fan Yining
CeO 2 -supported Au and Pd nanocatalyst (Au-Pd/CeO 2 ) was developed and used in the oxidation of 1,2-propanediol (1,2-PDO). Notably, by tuning catalyst composition and reaction conditions, the product selectivity could be well controlled to produce lactic acid (LA) majorly, which was one of the top twelve bio-based platform molecules with very broad application scopes. The catalyst with Pd/(Au + Pd) molar ratio at 0.25 should be the preferable catalyst was screened out to be preferable, affording LA in 92.0% selectivity, while 88.0% of 1,2-PDO was converted under mild reaction conditions (0.3 MPa of O 2 at 80 °C for 3 h). The superior catalytic activities of Au-Pd/CeO 2 probably attributed to the strong interactions between Au and Pd nano particles (NPs), as being reflected by High resolution transmission electron microscopy (HRTEM) and X-ray photoelectron spectra (XPS) characterizations. Moreover, strong interactions between Au and Pd NPs making it easy to generate active oxygen species. Superoxide radicals can oxide the first hydroxyl group of 1,2-PDO to carboxyl group, while H 2 O 2 can easy caused C-C bond breaks and generate unwanted by-products. Graphical The alternative text for this image may have been generated using AI.
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高影响因子
JOURNAL OF MEDICINAL CHEMISTRY
·
2021
·
IF 7.446
Yiqiang OuYang,Jian Gao,Lei Zhao,Junfeng Lu,Haiqing Zhong,Hua Tang,Shuanglong Jin,Lu Yue,Yuezhen Li,Wenjie Guo,Qiang Xu,Yisheng Lai
Two series of novel o-(biphenyl-3-ylmethoxy)nitrophenyl compounds (A1–31 and B1–17) were designed as programmed cell death protein 1 (PD-1)/PD-ligand 1 (PD-L1) inhibitors. All compounds showed significant inhibitory activity with IC50 values ranging from 2.7 to 87.4 nM except compound A17, and compound B2 displayed the best activity. Further experiments showed that B2 bound to the PD-L1 protein without obvious toxicity in Lewis lung carcinoma (LLC) cells. Furthermore, B2 significantly promoted interferon-gamma secretion in a dose-dependent manner in vitro and in vivo. Especially, B2 exhibited potent in vivo anticancer efficacy in an LLC-bearing allograft mouse model at a low dose of 5 mg/kg, which was more active than BMS-1018 (tumor growth inhibition rate: 48.5% vs 17.8%). A panel of immunohistochemistry and flow cytometry assays demonstrated that B2 effectively counteracted PD-1-induced immunosuppression in the tumor microenvironment, thereby triggering antitumor immunity. These results indicate that B2 is a promising PD-1/PD-L1 inhibitor worthy of further development.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Guofu Huang,Mianmian Wang,Yongyou Hu,Jianhua Cheng,Sihao Lv,Kui Yang
As a typical congener of Polybrominated diphenyl ethers (PBDEs), 2,2′,4,4′-tetrabromodiphenyl ether (BDE47) has attracted more and more attention due to its high biological toxicity and environmental abundance. In this study, a novel polyanionic cellulose stabilized Pd/Fe (PAC-Pd/Fe) nanoparticle was successfully synthesized for BDE47 degradation under ambient condition. Batch experiments showed that BDE47 degradation followed pseudo first-order kinetic model. Pd loading played a crucial role as it affected the formation of activated hydrogen species H ∗ and accelerated electron transfer. At Pd loading of 0.3 wt%, nearly 100% BDE47 was degraded completely within 10 min by 0.4 g L −1 PAC-Pd/Fe nanoparticles. When compared with strong acidic (pH 3) and alkaline (pH 9 and 11) conditions, weak acidic condition (pH 5) was more favorable for BDE47 degradation, with nearly 100% BDE47 was removed within 7.5 min. In the presence of HA inhibited the degradation of BDE47, and the degradation efficiencies within 15 min decreased from 100%, 88.6%, 79.5% to 73.1% as HA concentration increased from 0, 10, 40 to 70 mg L −1 . The degradation of BDE47 by PAC-Pd/Fe nanoparticles was a reductive debromination process, and a stepwise debromination from n-Br to (n-1)-Br BDEs was the dominant reaction, in which the para -Br was more susceptible to remove than ortho -Br. This study suggests PAC-Pd/Fe nanoparticle can be utilized as a promising remediation technology for PBDEs contaminated wastewater.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Chunfeng Mao,Kai Yin,Chenghan Yang,Guomeng Dong,Guokai Tian,Yiwei Zhang,Yuming Zhou
Controlling the spatial confinement effect and highly dispersed Pd nanoparticles (NPs) can help to improve applicability in catalysis, energy conversion, and separation. However, the nonspatial confinement effect, agglomeration of Pd NPs of catalyst and harsh reaction conditions have become the urgent problems to be solved in Suzuki-Miyaura cross-coupling reaction. Herein, we report the first application of a new MOFs@COFs by using core with metal organic frameworks (MOFs) NH 2 -MIL-101(Fe) and shell with covalent organic frameworks (COFs) for loading Pd NPs. The quickly formation of a transition state, the highly dispersed Pd NPs and the advancedly spatial confinement effect were achieved by coupling Fe base synergistic active components, electron-oriented anchoring with controlling pore scale, respectively. Most notably, as a proof-of-concept application, the high catalytic activity of NH 2 -MIL-101(Fe)@Pd@COFs( 3 + 3 ) in catalysis is elucidated for Suzuki-Miyaura coupling reaction by the broad scope of the reactants and the preeminent yields of the products, together with excellent stability and recoverability. With this strategy, the mechanism of Suzuki-Miyaura coupling reaction was verified by examining the catalytic activity. We hope that our approach can further facilitate the study of the design and use of functional MOFs@Pd@COFs materials.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xin Song,Mingyi Li,Jiaqi Xiong,Fangjun Shao,Zhongzhe Wei,Wenjuan Fang,Jianguo Wang
The carboxylation of alkynes with CO 2 is a pivotal reaction in organic synthesis. However, the generally poor adsorption and activation of CO 2 in heterogeneous catalytic systems have become a bottleneck problem restricting the efficiency of carboxylation reactions. In this study, we proposed a strategy for modifying heterogeneous catalysts with ionic liquid. By utilizing amino acid ionic liquids to modify the Pd/In 2 O 3 catalyst, the electronic structure of palladium (Pd) nanoparticles is optimized, and the adsorption and activation of CO 2 on the catalyst is enhanced. Additionally, the h-In 2 O 3 support not only regulates the electronic structure of Pd nanoparticles but also provides abundant oxygen vacancies, which facilitates the adsorption of CO 2 in the system. Due to the synergistic catalytic effects of the amino acid ionic liquid and the oxygen vacancies in the h-In 2 O 3 support, the Pd/h-In 2 O 3 -BmimPro catalyst demonstrates a remarkable phenylpropiolic acid yield of 93 % under mild conditions (50 °C, 0.5 MPa). This study provides valuable insights into the application of ionic liquid-modified catalysts in CO 2 conversion technologies.
研究领域:
催化化学
·
有机合成
·
二氧化碳利用
·
材料化学
·
绿色化学
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高影响因子
RUSSIAN JOURNAL OF ELECTROCHEMISTRY
·
2012
·Vol. 48
·期 11
·1135-1139
·
IF 0.534
Sun Xuping,Liao Fang,Lu Wenbo,Chang Guohui
In this paper, electrodeposition technique, in combination with well-established microfabrication techniques, is used for the first time herein to the controllable fabrication of novel Pd nanotextured micro-electrodes (NTMEs). This NTMES system is proven to be particularly powerful and versatile with two degrees of freedom: nanoscale control of electrode nanotexturing and the microscale control of the electrode size and shape.
研究领域:
生物医学工程
·
纳米医学
·
电化学传感
·
微系统技术
·
分子诊断
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高影响因子
CERAMICS INTERNATIONAL
·
2019
·Vol. 45
·期 10
·13150-13157
·
IF 3.45
Yan Wang,Xiaoning Meng,Mengxia Yao,Guang Sun,Zhanying Zhang
In this paper, pristine ZnO and Pd modified ZnO nanosheets have been successfully prepared via a facile hydrothermal route and the subsequent calcination process. The composition, morphology and nanostructure of the as-obtained materials were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM). The methane (CH 4 ) sensing properties of Pd/ZnO were compared with those of pure ZnO , and the materials showed the noticeable sensing capability when the loading amount of Pd was 1 at%. Moreover, the optimal working temperature of ZnO was reduced from 240 °C to 200 °C after loading Pd. The synthesized 1% Pd/ZnO nanocomposites not only showed the maximum response value 19.20 toward 5000 ppm CH 4 at 200 °C, but also exhibited the excellent selectivity and good repeatability. The improvement of CH 4 sensing performance by Pd nanoparticles could be attributed to the synergy effect with the spill-over effect and the nano-Schottky barriers.
研究领域:
材料科学
·
纳米科技
·
传感器技术
·
表面化学
·
半导体材料
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高影响因子
JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2018
·Vol. 18
·期 12
·8276-8281
·
IF 1.354
He Jieting,Wang Tianran,Qi Weihong,Li Yejun
Marks decahedral nanoparticles have attracted significant attention in recent years. In this work, a method of synthesizing Marks decahedron via etching regular decahedral nanoparticles is proposed and verified by Pd nanoparticles, which shows a high yield of Marks decahedron. The present
work suggests that one can tune the concave size of Marks decahedral via controlling the etching time and the amount of Poly(vinyl pyrrolidone) (PVP). The thermal stability of Marks nanoparticles is explained by Bond-Energy model, which predicts the largest groove to be the most stable configuration.
Moreover, the present method can be extended to synthesize Marks decahedral nanoparticles of other elements, and is of great significance for further studies and applications of Mark decahedral nanoparticles.
研究领域:
纳米材料
·
纳米粒子合成
·
物理化学
·
材料科学
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高影响因子
Materials
·
2024
·Vol. 17
·期 13
·3058
·
IF 3.1
Ziyue Wang,Ying Zhang,Hao Zhang,Qingdi Sun,Xiaohui He,Hongbing Ji
As worldwide plastic pollution continues to rise, innovative ideas for effective reuse and recycling of waste plastic are needed. Single-atom catalysts (SACs), which are known for their high activity and selectivity, present unique advantages in facilitating plastic degradation and conversion. Waste plastic can be used as a support or raw material to create SACs, which reduces waste generation while simultaneously utilizing waste as a resource. This work successfully utilized waste plastic polyurethane (PU) as a support, through a unique Rapid Thermal Processing Reactor (RTPR) to synthesize an efficient Pd1/PU SACs. At 25 °C and 0.5 MPa H2, Pd1/PU displayed outstanding activity and selectivity in the hydrogenation of styrene, as well as remarkable stability. Pd1/PU performed well in hydrogenating a variety of common substrates. These findings highlight the great potential of SACs in plastic waste reuse and recycling, offering intriguing solutions to the global plastic pollution problem.
研究领域:
环境科学
·
催化化学
·
材料科学
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高影响因子
危险品化学品经营许可证（带存储）