Cell Reports Physical Science
·
2025
·
IF 7.3
Zhongzhe Wei,Xu Liu,Mingxuan Wang,Yao Lv,Songtao Huang,Jing Wang,Ming Jiang,Zhixiang Yang,Zihao Yao,Sheng Dai,Xiaonian Li,Jianguo Wang
The semi-hydrogenation of alkynes represents a paramount chemical transformation in the synthesis of fine chemicals and pharmaceuticals. However, the structural evolution of active sites during the reaction remains elusive. Here, we constructed a self-adaptive Pd/Nb 2 O 5 catalyst for efficient semi-hydrogenation of alkynes. Mechanistic studies disclose that Pd/Nb 2 O 5 intelligently modulates its structure in response to the specific alkyne type, efficiently preventing Pd poisoning by weakening the strong adsorption of alkynes. During the hydrogenation of aliphatic alkynes, the Pd/Nb 2 O 5 interface undergoes dynamic changes, generating oxygen vacancies (O v ) in situ through hydrogen spillover. In contrast, for the case of reactants of aromatic alkynes, the interface sites remain relatively stable. Coverage-dependent kinetics reveal that the dynamic O v formation of Pd/Nb 2 O 5 is determined by the distinct adsorption mechanism of aromatic and aliphatic alkynes. Due to the evolving interface, Pd/Nb 2 O 5 exhibits a high turnover frequency value of 55,338 h −1 , breaking the linear scaling relationships.
研究领域:
催化
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化学反应工程
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材料科学
·
有机合成
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 24
·10388-10398
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IF 3.553
Zhong Mingjun,Zhang Shizhen,Dong Anwang,Sui Zhuyin,Feng Lijuan,Chen Qi
Heterogeneous metal–organic framework composites are widely used to catalyze the synthesis reaction of organic materials. Here, we report the use of a heterogeneous catalyst to catalyze the reaction of alcohols and amines to synthesize imines directly using a one-pot method. A low-dimensional Cu-MOF prepared by a simple surfactant-assisted method shows the morphology of nanorods. Cu-MOF nanorods provide an ideal support for preparing supported metal nanocatalysts. A reduction method was applied to immobilize the ultrafine noble metal Au and Pd nanoparticles on the surface of Cu-MOF nanorods to form a Cu-MOF/Au–Pd composite catalyst. Cu-MOF/Au–Pd catalyst is used to catalyze the reaction between alcohols and amines to form imines. Due to the synergy between different metal nanoparticles, it can effectively catalyze the reaction to form imines. In addition, Cu 2+ in Cu-MOF/Au–Pd catalyst facilitates the adsorption of substances by excess electrons and promotes product formation. After 12 h of catalytic reaction, the yield of imine is as high as 95%.
研究领域:
催化
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材料科学
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化学工程
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DOI
高影响因子
BIORESOURCE TECHNOLOGY
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2025
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IF 9
Jian Gao,Jingyu Wu,Yuancai Chen
This study found that bio-Pd 0 nanoparticles could launch proton motive force (PMF)-mediated antibiotics efflux pump (AEP) to confer the detoxification capability on Citrobacter freundii , as evidenced by the highest sulfamethoxazole (SMX) specific degradation rate (81.7 μg L −1 mg −1 protein d −1 ) at high PMF (pH 6). The batch experiment and RT-qPCR results indicated that bio-Pd 0 activated the AcrB efflux pump through upregulating the AEP transcriptional regulation factor ramA (2.7–3.1 times), which benefited the intra/extracellular respiration and ATP production/utilization. Path analysis revealed that the prosperity of metabolic activity and extracellular electron output capacity enabled SMX biodegradation, mainly through the electron redistribution and energy optimization with the formate dehydrogenase/hydrogenase based Short-chain (FDH/Hase-S-chain). The upregulation of hypE (2.7–8.6 times) and atpD (1.9–2.3 times) genes encoding the Hase respiratory chain and the F-type ATP synthase, respectively, further supports this mechanism. These novel findings provided a new strategy to improve the biodegradation efficiency of antibiotics wastewater.
研究领域:
微生物学
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环境科学
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产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 6
·1786-1796
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IF 2.936
Zhao Wei,Zhang Hongyi,Zhang Lei,Gong Jianchao,Chen Tianen,Ren Liming,Ji Yaxiong,Meng Fanbin
The methanol oxidation reaction is a promising route to eliminating trace amount of methanol in exhaust gases which aroused serious environmental concern. In this work, a novel Pd/MgAl 2 O 4 catalyst was prepared to construct the metal-support interface and employed in the methanol oxidation reaction. The reaction results show that the Pd/MgAl 2 O 4 catalyst could achieve 100% methanol oxidation at 198 ℃ over the Pd/MgO and Pd/Al 2 O 3 catalysts. The high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), CO-chemisorption, H 2 temperature programmed reduction (H 2 -TPR), and CO diffuse reflectance infrared Fourier transformed spectroscopy (CO-DRIFTS) show that the Pd was uniformly distributed over the MgAl 2 O 4 support due to strong interaction between Pd and MgAl 2 O 4 . The mechanism studies show that the abundant Pd-MgAl 2 O 4 interfaces significantly contributed to the reaction enhancement. The Pd-MgAl 2 O 4 interfaces could greatly enhance the oxidation reaction at a lower temperature with the assistance of oxygen vacancies compared with traditional oxide catalysts, which was confirmed by methanol temperature program surface reaction (MeOH-TPSR) experiments. In-situ DRIFTS is carried out to elucidate the reaction mechanism and establish the structure − activity relationship: the methanol could be effectively absorbed on the MgAl 2 O 4 support with oxygen vacancies to form bidentate formate, then the Pd species assisted the intermediates converting to CO 2 product. The Pd/MgAl 2 O 4 catalyst and its enhancement mechanism investigation provided a potential strategy in the VOCs removal catalysis development. Graphical Abstract
研究领域:
催化化学
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环境科学
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产品关联
DOI
高影响因子
SENSORS
·
2024
·Vol. 24
·期 7
·2110
·
IF 3.4
Yinfeng Shen,Yiping Liu,Chao Fan,Qudong Wang,Ming Li,Zhi Yang,Liming Gao
The mature processes of metal oxide semiconductors (MOS) have attracted considerable interest. However, the low sensitivity of metal oxide semiconductor gas sensors is still challenging, and constrains its practical applications. Bimetallic nanoparticles are of interest owing to their excellent catalytic properties. This excellent feature of bimetallic nanoparticles can solve the problems existing in MOS gas sensors, such as the low response, high operating temperature and slow response time. To enhance acetone sensing performance, we successfully synthesized Au-Pd/ZnO nanorods. In this work, we discovered that Au-Pd nanoparticles modified on ZnO nanorods can remarkably enhance sensor response. The Au-Pd/ZnO gas sensor has long-term stability and an excellent response/recovery process. This excellent sensing performance is attributed to the synergistic catalytic effect of bimetallic AuPd nanoparticles. Moreover, the electronic and chemical sensitization of noble metals also makes a great contribution. This work presents a simple method for preparing Au-Pd/ZnO nanorods and provides a new solution for the detection of acetone based on metal oxide semiconductor.
研究领域:
材料科学
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传感器技术
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sensors
·
2024
·
IF 8.2
Chengming Sui,Mingxue Zhang,Yueyue Li,Yilin Wang,Yuanzhen Liu,Ziqi Liu,Jihao Bai,Fengmin Liu,Geyu Lu
Bimetallic nanocrystals (NCs) have obtained significant attention due to their unique advantages of the intrinsic properties of individual metals and synergistic enhancements resulting from the electronic coupling between two constituent metals. In this work, Pd@Pt core–shell NCs were prepared through a facile one-pot solution-phase method, which had excellent dispersion and uniform size. Concurrently, ZnO nanosheets were prepared via a hydrothermal method. To explore their potential in nitrogen dioxide (NO2) gas sensing applications, sensitive materials based on ZnO nanosheets with varying mass percentages of Pd@Pt NCs were generated through an impregnation process. The sensor based on 0.3 wt % Pd@Pt-ZnO exhibited remarkable performance, demonstrating a substantial response (Rg/Ra = 60.3) to 50 ppb of NO2 at a low operating temperature of 80 °C. Notably, this sensor reached an outstanding low detection limit of 300 ppt. The enhancement in gas sensing capabilities can be attributed to the sensitization and synergistic effects imparted by the exceptional catalytic activity of Pd@Pt NCs, which significantly promoted the reaction. This research introduces a novel approach for the utilization of core–shell structured bimetallic nanocrystals as modifiers in metal-oxide-semiconductor (MOS) materials for NO2 detection.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Yufei Bao,Hui Liu,Zong Liu,Fulong Wang,Ligang Feng
Thermal annealing is usually employed for performance enhancement of catalysts while the reason is still unclear. Herein, performance improvement of a promising Pd/FeP system via thermal annealing to provide enhanced active sites, as a proof of concept, was demonstrated for the formic acid oxidation reaction. Two kinds of active sites of Pd and Pd@FeP were indicated in Pd/FeP catalyst by the well-recognized CO stripping technique; the low active/unstable Pd sites could be transformed into more active Pd@FeP sites via thermal annealing and electrochemical reduction. The best catalytic activity of annealed Pd/FeP catalyst was 1.6 times of fresh Pd/FeP and 2.8 times of Pd/C catalysts. A maximum catalytic efficiency increased by 65 % was revealed owing to the Pd@FeP active sites formation; as high as 55 % of the initial current was maintained after the accelerated stability test for 1000 cycles. The result helps understand the thermal annealing effect on electro-catalyst performance improvement.
研究领域:
材料科学
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电化学
·
催化工程
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-18
·
IF 14.7
Tang Xudong,Shang Yangyang,Yang Hong,Song Yalan,Li Shan,Qin Yusi,Song Jingyi,Chen Kang,Liu Yang,Zhang Dinglin,Chen Lei
The PD-1/PD-L1 pathway in mucosal immunity is currently actively explored and considered as a target for inflammatory bowel disease (IBD) treatment. However, systemic PD-L1 administration may cause unpredictable adverse effects due to immunosuppression. Here we show that reactive oxygen species (ROS)-responsive nanoparticles enhance the efficacy and safety of PD-L1 in a mouse colitis model. The nanoparticles control the accumulation and release of PD-L1 fused to Fc (PD-L1-Fc) at inflammatory sites in the colon. The nanotherapeutics shows superiority in alleviating inflammatory symptoms over systemic PD-L1-Fc administration and mitigates the adverse effects of PD-L1-Fc administration. The nanoparticles-formulated PD-L1-Fc affects production of proinflammatory and anti-inflammatory cytokines, attenuates the infiltration of macrophages, neutrophils, and dendritic cells, increases the frequencies of Treg, Th1 and Tfh cells, reshapes the gut microbiota composition; and increases short-chain fatty acid production. In summary, PD-L1-Fc-decorated nanoparticles may provide an effective and safe strategy for the targeted treatment of IBD.
研究领域:
药理学
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免疫学
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纳米技术
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胃肠病学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Zeyu Wang,Luyao Dai,Jiachao Yao,Tianjiao Guo,Dzmitry Hrynsphan,Savitskaya Tatsiana,Jun Chen
Multi walled carbon nanotubes (MWCNTs) have attracted more and more attention as adsorbents due to their excellent adsorption properties. By loading metal particles on MWCNTs, the chemical reduction ability of adsorbed pollutants could be provided, so as to achieve the purpose of adsorption and degradation of pollutants. Therefore, the removal process of NO 3 − -N by Fe–Pd–Fe 3 O 4 /MWCNTs was studied, including rapid adsorption of initial pollutants, gradual reduction of intermediate products and re-adsorption of final products. The results showed that Fe–Pd–Fe 3 O 4 /MWCNTs completely removed NO 3 − -N within 2 h, 39% and 25% of which were converted into NO 2 − -N and NH 4 + -N. The adsorption efficiency, kinetics, capacity and adsorption energy all followed the order of NH 4 + -N > NO 2 − -N > NO 3 − -N. With the recoverability and reusability of Fe–Pd–Fe 3 O 4 /MWCNTs having been confirmed in 5 consecutive cycles, the removal rate of NO 3 − -N still reached 43%. It has been shown that MWCNTs prolonged the reducing power for NO 3 − -N, due to avoiding the aggregation of metal particles. The rapid adsorption of initial pollutants, effective stepwise reduction and convenient recovery processes were of great value for the rehabilitation of polluted water.
研究领域:
环境科学
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材料科学
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水处理技术
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wenwen Song,Yanqi Xu,Xiangli Xie,Cunjun Li,Wenfeng Zhu,Qiankun Xiang,Wei Chen,Ningli Tang,Linjiang Wang
Electrocatalytic efficiency and stability have emerged as critical issues in the ethanol oxidation reaction (EOR) of direct ethanol fuel cells. In this paper, Pd/Co1Fe3–LDH/NF as an electrocatalyst for EOR was prepared by a two-step synthetic strategy. Metal–oxygen bonds formed between Pd nanoparticles and Co1Fe3–LDH/NF guaranteed structural stability and adequate surface-active site exposure. More importantly, the charge transfer of the formed Pd–O–Co(Fe) bridge could effectively modulate the electrical structure of hybrids, improving the facilitated absorption of OH– radicals and oxidation of COads. Benefiting from the interfacial interaction, exposed active sites, and structural stability, the observed specific activity for Pd/Co1Fe3–LDH/NF (17.46 mA cm–2) was 97 and 73 times higher than those of commercial Pd/C (20%) (0.18 mA cm–2) and Pt/C (20%) (0.24 mA cm–2), respectively. Besides, the jf/jr ratio representing the resistance to catalyst poisoning was 1.92 in the Pd/Co1Fe3–LDH/NF catalytic system. These results provide insights into optimizing the electronic interaction between metals and the support of electrocatalysts for EOR.
研究领域:
材料科学
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电化学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 26
·21337-21344
·
IF 3.289
Hong Jiang,Songlin Xue,Yefei Liu,Rizhi Chen,Weihong Xing
The Pd@ZIF-L catalysts with uniform crosshair-star shape and a size of about 20 μm were fabricated by an assembly method that enables the crystallization of ZIF-L in water with the presence of polyvinylpyrrolidone (PVP)-stabilized Pd nanoparticles (NPs). The physical and catalytic properties of the Pd@ZIF-L catalysts are greatly affected by the molar ratios of 2-methylimidazole (2-MeIM)/Zn2+ and PVP/Zn2+. Their catalytic activities were evaluated by the catalytic reduction of p-nitrophenol to p-aminophenol. The results indicate that a lower molar ratio of 2-MeIM/Zn2+ is beneficial for the increase of Pd loading and p-nitrophenol conversion, but a suitable molar ratio (≥20) of 2-MeIM/Zn2+ is helpful to the crystallization of ZIF-L and the encapsulation of the Pd NPs within the ZIF-L framework. The Pd@ZIF-L catalyst synthesized at a lower PVP/Zn2+ molar ratio has higher Pd loading and p-nitrophenol conversion due to the easy adsorption of PVP–Pd NPs onto the ZIF-L surfaces. This work would aid the development of high-performance Pd@ZIF-L catalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
HYDROMETALLURGY
·
2019
·
IF 3.465
Shunyan Ning,Shichang Zhang,Wei Zhang,Jie Zhou,Siyi Wang,Xinpeng Wang,Yuezhou Wei
The separation of fission products Ru, Rh, and Pd will benefit both the nuclear fuel cycle and enlarge the platinum group metals source. A silica-based iso Bu-BTP/SiO 2 -P adsorbent was used to separate Ru, Rh, and Pd from nitrate solution. It exhibited good adsorption towards Ru, Rh, and Pd with the uptake rates over 95% at 55 °C in 0.1 M HNO 3 –3 M NaNO 3 solution and no adsorption towards 238 U(VI). The adsorption towards Ru, Rh, and Pd matched well with pseudo-second-order model with the equilibrium obtained within 24 h, 24 h and 0.5 h and Langmuir adsorption isotherm model with the saturation adsorption amounts as high as 0.37 mmol/g, 0.34 mmol/g and 0.71 mmol/g respectively. The adsorbed Pd, Rh, and Ru can be desorbed by 0.1 M HNO 3 –0.1 M thiourea , 2 M HCl and NaClO solution (CP) which is expected to realize their mutual separation in desorption stage using the above-mentioned eluents successively. Both FT-IR and XPS revealed that C N C played key role during adsorption and the adsorption needed the participation of NO 3 − to keep charge balance. In a word, iso Bu-BTP/SiO 2 -P is a promising adsorbent for separation and recovery Ru, Rh, and Pd, especially in the case of separating them from other fission products and actinides from high level liquid waste .
研究领域:
核化学
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材料科学
·
放射化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）