Chemistry-An Asian Journal
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2022
·Vol. 17
·期 24
·e202200993
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IF 4.839
Zhijie Zhu,Xu Hu,Xingda An,Mengqi Xiao,Liang Zhang,Chaoran Li,Le He
Graphical The influence of the composition of bimetallic nanocrystals on their performance of photothermal catalytic CO 2 hydrogenation was investigated. Pd and Ni play different roles in the photothermal catalytic processes in the bimetallic system, which leads to a functional tradeoff over the stoichiometric ratio. Bimetallic nanomaterials exhibit excellent catalytic performance in photothermal CO 2 hydrogenation due to the synergistic effect between the two metal components. However, the component-performance relationship remains unclear, which hinders the design of efficient bimetallic catalysts and the investigation of catalytic reaction mechanism. Here we illustrate the influence of the composition of binary alloy on their performance of photothermal catalytic CO 2 hydrogenation by using monodispersed Pd−Ni nanocrystal as an example. Our study reveals that Ni and Pd play a significantly different role in the catalytic processes. Higher Ni component in the catalysts could lead to stronger light absorption, higher activity, and lower CO selectivity. The optimized Pd 4 Ni 1 −SiO 2 catalyst exhibited a near-unity and stable CO production rate of 230 mmol ⋅ g −1 ⋅ h −1 under 25-sun illumination. This study paves the way for the usage of bimetal in photothermal CO 2 catalysis towards more efficient solar-to-chemical energy conversions, and sheds light on some general design principles of bimetallic catalysts to balance the intrinsic properties of individual components.
研究领域:
材料科学
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催化化学
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能源转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CARBON
·
2022
·
IF 11.307
Xiang Yu,Yue Zhan,Tingting Fan,Yuqi Zhang,Shunqin Liang,Limin Sun,Xiaoli Hu,Weiping Fang,Zhou Chen,Xiaodong Yi
The stabilization and transport of the reactants, intermediates and products are significant to rational design of an industrial catalyst. In this work, we encapsulated the surface of Pd/g-C 3 N 4 catalyst with acrylic acid (AA) using a photo-induced grafting method to mimic the 3-dimensional nature of enzymes. A combined characterization and ab initio calculation revealed that AA ligands on the surface controlled the adsorption and diffusion behaviors of the reactants, rather than alter the electronic or geometric properties of Pd active centers. The optimized catalyst (Pd/CNA-4) significantly enhances isoprene partial hydrogenation activity without a decline in semi-hydrogenation selectivity. This approach can be further optimized by changing the types of the encapsulating ligands and can meet other specific catalytic reactions to regulate their conversion and selectivity and is therefore expected to extend to other areas of heterogeneous catalysis .
研究领域:
催化化学
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材料科学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2017
·
IF 3.204
Qifu Huang,Wenzhi Li,Qizhao Lin,Xusheng Zheng,Haibin Pan,Dong Pi,Chunyu Shao,Chao Hu,Haitao Zhang
In this paper, the catalyst of Pd–NiCo 2 O 4 /SiO 2 was prepared and applied to the catalytic combustion of lean methane. Pd and NiCo 2 O 4 nanoparticles were uniformly distributed on the SiO 2 support, so that every Pd or NiCo 2 O 4 nanoparticle was separated from each other by another component. Comparing with Co 3 O 4 /SiO 2 , NiCo 2 O 4 /SiO 2 , Pd–Co 3 O 4 /SiO 2 and Pd#NiCo 2 O 4 /SiO 2 (catalysts without uniform distribution of Pd and NiCo 2 O 4 nanoparticles), Pd–NiCo 2 O 4 /SiO 2 had the highest catalytic activity in the catalytic combustion of lean methane, with a methane total conversion temperature at 378 °C. In addition, the high activity did not decrease during the long time reaction, which showed good thermal stability . TEM and BET results showed that the nanoparticle sizes of Pd and NiCo 2 O 4 were very small. The XRD patterns indicated that the Pd nanoparticles were highly dispersed on the surface of SiO 2 . The XPS spectra demonstrated the formation of NiCO 2 O 4 , the presence of enough active oxygen species on the catalyst surface and the high ratio of PdO/Pd 0 . The enhanced influence of Ni introduction was also proved by comparison tests. All these results indicated that the high catalytic activity of Pd–NiCo 2 O 4 /SiO 2 mainly comes from the nanoparticle distribution and the Ni cation enhancement.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2020
·Vol. 95
·期 9
·2403-2410
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IF 2.75
Li Sun,Chuanliang Li,Hua Zhang,Binlin Dou,Wenxian Su,Lixin Zhang
BACKGROUND At present, much attention has been focused on the development of methane (CH 4 ) sensors due to a series of explosions and fires caused by CH 4 gas leakage. RESULTS Here, a CH 4 thermoelectric gas sensor (TGS) was fabricated by fixing 3D porous palladium/cobalt oxide (Pd/Co 3 O 4 ) catalyst on a commercial thermoelectric module. 3D porous Pd/Co 3 O 4 catalysts were prepared by a co-precipitation and gel-casting method. The pore structure in catalysts could be tailored only by adjusting the gel viscosity during the formation process. The protocol to tune the pore structure is facile and effective for the improvement of the activity of catalysts. By means of various techniques, the catalysts were characterized and then the possible catalytic mechanism was revealed. The CH 4 TGS based on the optimal Pd/Co 3 O 4 catalyst began to respond at 200 °C, following an obvious output voltage (Δ V ) of 5 mV. Enhancing the operating temperature to 240 °C, the value of Δ V reached to 31 mV and exhibited a linear relationship with CH 4 gas concentration. Meanwhile, the CH 4 TGS showed high sensitivity, repeatability and stability. CONCLUSION The easy and effective preparation method presented to prepare 3D porous Pd/Co 3 O 4 catalyst can provide an unique perspective on the development of 3D porous materials with excellent properties. It can be anticipated that the CH 4 TGS based on the 3D porous Pd/Co 3 O 4 catalyst will be a potential candidate for the detection of CH 4 gas in industrial settings. © 2020 Society of Chemical Industry
研究领域:
材料科学
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化学工程
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传感器技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Jun Zhang,Lanyu Luo,Jiankun Wang,Xinlan Xu,Tiantian Peng,Boyu Liu,Lingying Jiang,Meng Jin,Weimin Wu,Laizheng Luo,Huan Yi,Shi-Yu Lu
Optimizing the electronic configuration presents a promising approach to enhance intrinsic activity and minimize noble metal use in direct methanol fuel cells (DMFCs). Metal–support interactions, commonly employed to induce interfacial charge redistribution, play a crucial role in this optimization. This study successfully synthesized a Pd/O-OMS-2 electrocatalyst characterized by Pd–O–Mn interfacial chemical bonds and Mn3+/Mn4+ redox couples, serving as a stable bifunctional catalyst for both the oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR). Unlike the mixed Pd–O/Mn bonds in Pd/O/Mn-OMS-2, the Pd–O–Mn bonds in Pd/O-OMS-2 not only enhance metal–support interactions and promote uniform dispersion of Pd nanoparticles but also facilitate electron transfer and the conversion between Mn3+ and Mn4+. These structural and compositional advantages endow the Pd/O-OMS-2 catalyst with superior ORR and MOR performance. The catalyst achieves a higher half-wave potential (E1/2) of 0.901 V, a mass activity of 0.937 A mgPd–1, and enhanced methanol permeability, outperforming Pd/O/Mn-OMS-2, Pd/OMS-2 and commercial Pd/C catalysts. Moreover, in an alkaline electrolyte, the Pd/O-OMS-2 catalyst follows a typical four-electron reaction pathway for ORR (O2 to H2O) and promotes faster reaction kinetics and charge transfer rates. In terms of durability, the Pd/O-OMS-2 catalyst exhibits minimal E1/2 decay (8 mV) and retains its structural integrity even after 10,000 cyclic voltammetry (CV) cycles. Additionally, it demonstrates the highest mass activity and stability during the MOR process. The exceptional ORR/MOR performance can be attributed to the synergistic effect of strong metal–support interactions, high Pd nanoparticle dispersion, and increased Mn3+ active species. The construction of interfacial chemical bonds offers a prospective strategy to optimize electronic configurations and develop advanced bifunctional electrocatalysts for ORR and MOR.
研究领域:
电化学
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催化材料
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能源材料
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2024
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IF 3.8
Zhenghua Zhang,Yang Tian,Wenjun Gao,Yubin Hu,Liangping Luo,Lichang Lei,Shasha Shen,Dan Han
Objectives: Immune checkpoint inhibitors (ICIs) have demonstrated potential in inhibiting the growth of malignant pleural mesothelioma (MPM), and their efficacy is associated with the expression of programmed death-ligand 1(PD-L1). This study evaluated a PD-L1-targeted nanoprobe for detecting PD-L1 expression in a nude mouse model of malignant pleural mesothelioma (MPM).Methods: A PD-L1-binding peptide (WL-12) was conjugated with superparamagnetic iron oxide nanoparticles (SPIONs) to create the nanoprobe WL-12@Fe₃O₄. The nanoprobe’s stability, biotoxicity, targeting ability, and in vivo magnetic resonance (MR) imaging effects were assessed and compared to non-targeted Fe₃O₄ nanoparticles. ΔT2 values and PD-L1 expression were measured in H226 and MSTO-211H tumor tissues over 4 weeks to analyze correlations.Results: The WL-12@Fe₃O₄ nanoprobe demonstrated uniform distribution and a spherical shape, with a larger size (43.82 nm) and lower surface potential (−9.34 ± 0.54 mV) compared to Fe₃O₄ (32.67 nm, −20.20 ± 0.88 mV, P < 0.05). The XPS and FT-IR analysis results indicate the successful coupling of WL-12 with Fe3O4. It was well dispersed in serum and saline and showed no cytotoxicity or organ damage in vivo. The probe selectively accumulated in PD-L1-expressing MPM cells, especially MSTO-211H, and exhibited significantly higher uptake in high PD-L1-expressing H460 cells (930.22 ± 11.75 ng/mL) compared to low PD-L1-expressing A549 cells (254.89 ± 17.33 ng/mL, P < 0.05). Tumor iron levels in the WL-12@Fe₃O₄ group were significantly elevated (141.02 ± 17.33 μg/g) compared to controls (36.43 ± 3.56 μg/g, P < 0.05), with no significant differences in other organs (P > 0.05). The T2 values of H226 and MSTO-211H tumors decreased after probe injection, with ΔT2 values significantly higher in the targeted group than the nontargeted group (P < 0.05). ΔT2 values increased over 4 weeks, correlating strongly with PD-L1 expression (P < 0.05).Conclusion: The PD-L1-targeted nanoprobe with MRI is a promising tool for noninvasive, real-time assessment of PD-L1 expression in MPM.
研究领域:
肿瘤学
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医学影像学
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纳米医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2018
·Vol. 10
·期 47
·22348-22356
·
IF 7.233
Xusheng Cheng,Dongxu Wang,Jiancong Liu,Xin Kang,Haijing Yan,Aiping Wu,Ying Gu,Chungui Tian,Honggang Fu
Decreasing Pd usage whilst maintaining a superior performance is promising, but remains a challenge in the catalytic field. Herein, we have demonstrated the highly efficient promotion of Mo2N with a reduced amount of Pd for the liquid-phase hydrogenation reaction. The Mo2N (2–3 nm) was uniformly anchored onto mesoporous SBA-15 by using PMo12 as the Mo source. The small size and good dispersion of Mo2N is favourable for allowing their effective contact with post-loading Pd. This good contact is conducive to developing a synergistic catalyst, which was verified by studying the liquid-phase hydrogenation of p-nitrophenol (PNP) to p-aminophenol (PAP) with NaBH4 as the H source. The conversion ability of PNP to PAP on 1 wt% Pd–Mo2N/SBA-15 was vastly superior to 1 wt% Pd/SBA-15 and even better than 20 wt% Pd/SBA-15. The low-Pd, highly efficient catalysis is ascribed to the transfer of the electrons from Mo2N to Pd for the easy activation of H. The synergy can be affected by the type of support used. SBA-15 is superior to SiO2 and the other supports, which could be related to the large surface area and the plentiful number of pores on SBA-15, which is favourable to the dispersion of Pd and Mo2N, and the transfer/diffusion of the reactants. In particular, a highly efficient catalyst can be achieved at an even more reduced Pd loading (0.05 wt%). The current method describes the design of a highly efficient catalyst for the hydrogenation reaction using low amounts of noble metals.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2017
·Vol. 19
·期 21
·5103-5113
·
IF 9.125
Ying Duan,Min Zheng,Dongmi Li,Dongsheng Deng,Lu-Fang Ma,Yanliang Yang
The catalytic conversion of HMF to 2-hydroxy-3-methyl-2-cyclopenten-1-one (MCP), which is a valuable edible essence that has traditionally been obtained from adipic acid, was achieved with an isolated yield of 58%. This procedure comprised two steps: the hydrogenation of 5-hydroxymethylfurfural (HMF) to 1-hydroxy-2,5-hexanedione (HHD) in water on Pd/Nb2O5 catalysts and then the isomerization of HHD to MCP in the presence of a base. The Nb2O5 supports, which were acidic, were characterized by FTIR, XRD and NH3-TPD. The supported Pd/Nb2O5 catalysts, in which Pd was highly dispersed, were synthesized employing cyclohexene as a reductant and were characterized by XRD, TEM, ICP-AES, XPS, EDX and CO pulse chemisorption. The high conversion of HMF was attributed to the high dispersion of Pd, and the acidity of the supports led to high selectivity for HHD. The conversion of HHD to MCP was an intramolecular aldol condensation reaction, and the protonic solvent favored this reaction. Ca–Al was proved to be an effective solid base for the conversion of HHD to MCP in water.
研究领域:
化学工程
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 10
·3609-3618
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IF 6.119
Palle Ramana Murthy,Jing-Cai Zhang,Wei-Zhen Li
Pd-Based catalysts are efficient for methane combustion but impractical at high temperatures due to the sintering effect. Herein, we report a thermally stable Pd/SBA-15 catalyst that was prepared by using the sol-immobilization (SI) method, instead of the conventional incipient wetness impregnation (IWI) method. Pd nanoparticles retain the small size of ∼5 nm in the channels of SBA-15 in Pd/SBA-15-SI even after aging at 800 °C in air for 3 days, while those in the Pd/SBA-15-IWI samples aggregate into particles larger than 10 nm over the surface. The thermally stable Pd/SBA-15-SI indeed displays excellent catalytic activity for methane combustion at low temperatures with T50 at ∼300 °C and T90 at ∼350 °C and high stability during cyclic operations, which are much superior to those of the Pd/SBA-15-IWI catalysts. Interestingly, hydrothermal treatment of the Pd/SBA-15-SI catalysts leads to partial re-dispersion of Pd to form smaller particles of ∼1.6 nm, while the catalytic activity decreases a bit. Steam in the reactant mixture has a negative effect on the catalytic activity of Pd/SBA-15-SI catalysts, presumably due to the competitive adsorption of H2O to O2/CH4. Significantly, the size of Pd nanoparticles is essential to the catalytic performance and those having sizes of ∼5 nm are the most active. Finally, the catalytic activity of the catalysts in the presence of CO2 was studied. This work might be helpful in designing stable metal catalysts using porous materials for reactions under harsh conditions.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
PHARMACOLOGICAL RESEARCH
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2022
·
IF 10.334
Qing Li,Meng-Sheng Deng,Ren-Tao Wang,Hao Luo,Yuan-Yuan Luo,Dong-Dong Zhang,Kui-Jun Chen,Xiao-Fu Cao,Guang-Ming Yang,Tie-Mei Zhao,Bo Xu,Cheng-Xiong Xu,Jian-Min Wang
Idiopathic pulmonary fibrosis (IPF) is a progressive disease with high mortality and limited therapeutic options. The immune checkpoint PD1/PD-L1 axis is related to the pathogenesis of pulmonary fibrosis, and upregulated expression levels of PD-L1 have been demonstrated in IPF patients. However, the mechanism of PD-L1 in pulmonary fibrosis is not fully understood. Here, we demonstrated upregulated expression of PD-L1 in fibrotic lung tissues and sera of IPF patients. Bleomycin (BLM) treatment induced PD-L1 upregulation, EMT (Epithelial-Mesenchymal Transition) and fibrosis-like morphology changes in human pulmonary alveolar epithelial cells (HPAEpiCs). Silencing PD-L1 attenuated BLM-induced EMT and fibrosis-like morphology changes in HPAEpiCs. In addition, we identified that PD-L1 directly binds to vimentin and inhibits vimentin ubiquitination, thereby increasing vimentin levels in HPAEpiCs. Silencing of vimentin inhibited BLM- and PD-L1-induced fibrosis in HPAEpiCs. The correlation between PD-L1 and EMT or vimentin expression was further confirmed in clinical samples and animal models. Finally, we used BLM- and paraquat-induced pulmonary fibrosis animal models to confirm the anti-pulmonary fibrosis effects of PD-L1 silencing. Taken together, our findings suggest that upregulated PD-L1 stimulates EMT of alveolar epithelial cells by increasing vimentin levels by inhibiting vimentin ubiquitination, thereby contributing to pulmonary fibrosis.
研究领域:
呼吸病学
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免疫学
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细胞生物学
✓ 已验证
DOI
PubMed
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2024
·
IF 7.2
Xiequan Chen,Qi Zhang,Song Li,Haiyong Wang,Xinghua Zhang,Lungang Chen,Longlong Ma,Jianguo Liu
Acidic promoters are significant in the hydrodeoxygenation (HDO) of bioderived furans into alkanes over metal-acid bifunctional catalysts. Here, a supported Pd/HPW-SiO 2 catalyst was prepared to investigate the promotion effect of phosphotungstic acid (HPW) on the HDO of HMF-acetone adduct (H-Ac). Characterizations suggested that an intimate contact between Pd and HPW was established in Pd/HPW-SiO 2 . HPW promoters significantly reduced the reduction temperature of Pd oxides with enhanced hydrogenation and HDO capability. Particularly, in-situ DRIFTS confirmed that Pd-HPW sites significantly weakened the π CO η 2 adsorption mode (ν 3 (C=O)) of C=O group on Pd surfaces. Thereby, the HDO efficiency was synergistically improved through releasing more Pd metal sites to activate hydrogen for hydrogenation and HDO with HPW promoters. Eventually, >90% yield of nonane was efficiently achieved at 160 °C. This work is applicable to explore the structure-activity relationship of bifunctional catalysts in the efficient HDO of complicated oxygenated bioderived furans.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
Advanced Energy and Sustainability Research
·
2024
·Vol. 5
·期 8
·2400044
·
IF 6.2
Jie Li,Jieying Cai,Yan Zhang,Peng Wang,Xuehai Wang,Xiangchen Fang,Yunbo Yu,Wenpo Shan
Mesoporous MgAl 2 O 4 is synthesized via a novel sol–gel combustion method and the concentration of oxygen defects on the surface is modulated through varying the calcination temperature (850, 900, 1000, and 1100 °C). Notably, the 1Pd/MgAl 2 O 4 -1000 catalyst exhibits superior catalytic activity and stability. The turnover frequency (TOF) for 1Pd/MgAl 2 O 4 -1000 is 0.079 and 0.058 s −1 under dry conditions (300 °C) and wet conditions (380 °C), respectively. The results of H 2 temperature-programmed reduction and X-Ray photoelectron spectroscopy reveal that the principal active species within the Pd/MgAl 2 O 4 -y catalyst is PdO. Specifically, the Pd–MgAl 2 O 4 -1000 catalyst exhibits the lowest temperature reduction peak (120 °C) and the highest redox capability. Additionally, O 2 temperature-programmed oxidation further elucidates that PdO x species in the Pd/MgAl 2 O 4 -1000 catalyst is prone to decomposition and the resultant palladium metal is readily reoxidized. Consequently, the rapidity of the redox cycle between PdO and Pd 0 emerges as a pivotal factor in CH 4 catalytic combustion. Furthermore, a correlation analysis among catalyst particle size, oxygen defect concentration, and TOF is conducted. The findings illustrate a distinct volcano-shaped curve in the relationship between oxygen defect concentration and TOF for the 1Pd/MgAl 2 O 4 −y catalysts. A comparable trend is also evident in the correlation between Pd particle size and TOF.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）