APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Qian Zhang,Yuanyu Shi,Xianjin Shi,Tingting Huang,Shuncheng Lee,Yu Huang,Jun-ji Cao
Photo-oxidative NO x removal often encountered with sluggish charge carrier separation kinetics and poor selectivity. Herein, Pd/ferroelectric Bi 4 Ti 3 O 12 nanoflakes (Pd/BTO NF) were constructed to investigate the photo-excited charge separation, O 2 activation and the generated reactive oxygen species (ROS) in dictating NO removal. Results showed that the depolarization field of ferroelectric BTO NF significantly promoted bulk charge separation, leading to boosted NO removal reaction kinetics (10 times higher) for Pd/BTO NF comparing with Pd/TiO 2 . Revealed by electronic paramagnetic resonance and radical scavenging tests, it is observed that the primary O 2 activation species differed among Pd, Ag and Pt supported BTO NF photocatalysts, which resulted in different selectivity. The underlying mechanism of NO photo-oxidative conversion pathway was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy. This work illustrate that metal/ferroelectric interfaces can be tuned to obtain differing O 2 activation species, and notable selectivity changes in photocatalysis mediated environmental remediation reactions.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2024
·
IF 3.7
Xin Li,Yue Ma,Xuning Wang,Jianguo Wu,Dong Cao,Daojian Cheng
The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd 0 /Pd 2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C 3 N 4 –300 catalyst with a Pd 0 /Pd 2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd 0 and Pd 2+ in Pd/g–C 3 N 4 –300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.
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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.
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Electrocatalysis
·
2024
·Vol. 15
·期 4
·281-290
·
IF 2.7
Xiang Qun,Wang Yizhong,Wang Shuang,Fu Xucheng,Gao Guiqi,Yan Ruiwen
In this work, the CeO 2 nanoparticles were dispersed onto the surface of graphene oxide (GO), followed by electrodeposition of Pt–Pd alloy nanoparticles on the CeO 2 surface to fabricate Pt–Pd@CeO 2 /graphene oxide composites (Pt–Pd@CeO 2 /GO). Morphological investigation was conducted using X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). The results of morphological characterization revealed that CeO 2 nanoparticles acted as cores, while Pt–Pd alloy nanoparticles formed shells. The electrocatalytic oxidation performance of Pt–Pd@CeO 2 /GO composites for methanol electro-oxidation reaction (MOR) was systematically investigated. The mass activity for MOR on Pt 1 Pd 1.3 @CeO 2 /GO electrocatalyst was 1128 mA·mg Pt+Pd −1 , which was 5.0-fold higher than that of Pt/C catalysts. The synergistic effect between Pt and Pd, along with the active oxygen-containing species of CeO 2 effectively enhanced catalytic activity. This work presents a novel approach to developing catalysts with high catalytic performance for MOR. Graphical Abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Chao Feng,Yuxi Bi,Chong Chen,Yunxia Wang,Shuangju Li,Yuan Pan,Hongchuan Xin,Yukun Lu,Fang Liu,Xuebing Li,Yunqi Liu,Runduo Zhang,Zhong Wang
Photothermal synergistic low-temperature catalytic volatile organic compounds (VOCs) degradation has an advantage on energy efficiency and reduction of carbon emissions. Herein, an impregnation-pyrolysis-oxidation strategy was adopted to synthesize Pd/Mn 3 O 4 heterojunction catalyst. Under photothermal synergistic conditions, 0.60Pd/Mn 3 O 4 catalyst exhibited an excellent activity for propane total oxidation, with a T 90 value of 219.1 ℃, which was 115.3 ℃ lower than that of Mn 3 O 4 . Enhancement effect of the heterojunction structure on photothermal synergy was detected by various characterization techniques and density functional theory calculation. The presence of Pd species enhanced the low-temperature reducibility of Mn 3 O 4 . Meanwhile, O 2 molecules were more easily activated at the Pd sites and overflow to the surface of Mn 3 O 4 for reaction. Besides, the formation of p-n junction between Pd species and Mn 3 O 4 in heterojunction structure promoted the charge separation and the migration of carriers, and boosted the generation of oxygen free radical, resulting in a significant improvement in photothermal catalytic activity. Overall, this study provided new strategy and deep insight for constructing heterojunction to enhance photothermal catalytic performance of VOC elimination.
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ChemSusChem
·
2025
·
IF 6.6
Qian Jiang,Zuzhi Li,Javier Remón,Hui Xin,Zhicheng Jiang,Bi Shi
Finding new catalytic applications for tannin, a biomass resource, exploiting its structural features and renewable nature, helps contribute toward carbon neutrality in catalysis. In this study, novel Pd-supported, carbon-neutral catalysts have been synthesized using tannic acid. First, tannic acid was cross-linked and coated on the surface of nano-SiO2. This material was then subjected to controllable carbonization, with the temperature being optimized, to obtain the catalyst support SiO2@TA-T (T: carbonization temperature). Experimental results demonstrated that carbonizing at 400 °C remained part of the phenolic hydroxyls of tannin with satisfactory reducing ability. Meanwhile, the condensation and the deoxygenation of tannin increased the thermal stability of this support and introduced porous structures and abundant defect sites. This material was then used to adsorb and in situ reduce Pd2+ to develop Pd-based catalysts. To this end, this synthesized Pd/SiO2@TA-400 catalyst was then used to hydrogenate vanillin, with a conversion of 99% to vanillyl alcohol at a pressure of 0.5 MPa initial H2 and a temperature of 20°C for 60 min. Such remarkable results were corroborated in the hydrogenation of several lignin-derived aromatic aldehydes, with our catalyst achieving high conversion and outstanding recyclability (5 recycles).
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Heying Li,Jingming Zhai,Qingnan Zhang,Jinghua Li
Infections resulting from bacteria resistant to antibiotics represent a significant risk to human health. Therefore, exploring novel and effective antibacterial treatment strategies as substitutes for traditional antibiotics is essential. Here, we developed heterogeneous bimetallic Pd@Pt Cubes with a core-shell structure for near-infrared light-enhanced bacterial infection treatment. Heterogeneous core-shell bimetallic Pd@Pt nanocubes demonstrated remarkable photothermal properties along with peroxidase-mimic activity, promoting the combined interaction between photothermal antibacterial therapy (PTT) and chemodynamic therapy (CDT). As demonstrated in vitro antibacterial tests, Pd@Pt Cubes can effectively eliminate both E. coli and S. aureus , and enhance drug penetration in biofilm by disrupting the biofilm. Furthermore, in vivo antibacterial tests indicated that Pd@Pt Cubes can significantly enhance the repair of tissues in bacterial infection sites. Overall, this study constructed an efficient and multifunctional antibacterial nanoplatform through a rational combination and design, and achieved PTT/CDT bimodal bacterial infection treatment through multiple enhancement strategies.
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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.
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Advanced Optical Materials
·
2025
·Vol. 13
·期 10
·2402968
·
IF 7.2
Lei Yao,Yunjia Wei,Xing Zhao,Xiangnan Zhu,Dexiang Chen,Xiao Tang,Xingce Fan,Teng Qiu,Qi Hao
Plasmonic catalysis employs nanomaterials to mediate the conversion of photon energy into localized electromagnetic fields, hot carriers, and thermal energy, facilitating molecular transformations under mild conditions. Understanding the mechanisms governing plasmonic effects is crucial for optimizing the yield and selectivity in plasmonic catalysis. However, challenges persist in elucidating the role of plasmonic field effects due to the complex interactions among various contributing mechanisms. This study introduces Au@Al 2 O 3 -Pd-Au@Al 2 O 3 trimer arrays to decouple plasmonic field effects from other influences. The alumina coating on the Au particles prevents charge transfer between gold and reactants, enabling focused examination of the field effects on Pd catalysts. Employing real-time monitoring with liquid-state surface-enhanced Raman scattering (SERS), this work investigates the catalytic efficiency and kinetics of the C─C coupling reactions on palladium by tuning the near-field strengths. Polarization-dependent studies reveal that strong near-field intensity around the trimer structures is amplified by ≈60-fold under optimized conditions. The findings offer insights for optimizing catalytic reaction conditions and designing more effective composite plasmonic catalysts.
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Acta Pharmaceutica Sinica B
·
2025
·
IF 14.6
Changyong Guo,Shipeng He,Huaxing Shen,Wei Cong,Jinqiu Li,Yajing Ji,Wenjing Huang,Fei Gao,Honggang Hu
Checkpoint blockade immunotherapy has emerged as a transformative approach in cancer treatment by activating tumor-infiltrating T cells. However, the efficacy of PD-L1 blockade is restricted in “cold” tumors, which are characterized by low immunogenicity, presenting a challenge to immunotherapy. This study introduces an innovative strategy, utilizing cathepsin-cleavable N -(2-hydroxypropyl) methacrylamide (HPMA) polymer-assisted combined photodynamic therapy (PDT) and PD-L1 degradation for the first time, effectively treating T cell-deficient tumors. The degradable main-chain polymer, conjugated with photosensitizer porphyrin, facilitates the accumulation of reactive oxygen species (ROS), triggering immunogenic cell death (ICD) and promoting cytotoxic T lymphocytes (CTLs) infiltration into tumors. Multivalent peptide antagonists of PD-L1 promote PD-L1 degradation in lysosomes through receptor crosslinking, overcoming the adaptive cycling of PD-L1 to the tumor cell surface. These findings demonstrate that polymer-assisted PDT and PD-L1 crosslinking degradation represent a potential novel strategy for anti-tumor immunotherapy, providing valuable tools for expanding immunotherapy applications in immunosuppressive cancers.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Xinyue Zhang,Yuan Yao,Yingying Cao,Xin Tan,Xiaomin Fang,Yanqiang Zhang
The high strain energy of the three-membered ring can increase the combustion calorific value of space fuels. At present, the cyclopropanation of alkenes is the bottleneck to obtain highly-energy three-member-ring fuels. In this article, Pd single-site catalysts (SSCs) were prepared to catalyze the cyclopropanation of norbornene. Pd2+ on the SSCs enhanced the adsorption of CH2N2 through electrostatic interaction, efficiently forming metal carbene. The conversion and selectivity of norbornene cyclopropanation reached 99.9% and 96.9%, which are much higher than those of commercial Pd/C (conversion 42.3%, selectivity 80.8%). In addition, the obtained tricyclooctane shows excellent properties (density 0.93 g/cm3, calorific value 42.75 MJ/kg) to be a promising high-performance rocket fuel. This work provides an efficient method for the synthesis of cyclopropane-based space fuels from alkenes.
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Scientific Reports
·
2021
·Vol. 11
·期 1
·1-9
·
IF 4.38
Yue Song,Sun Kexin,Li Siyuan,Liu Yi,Zhu Qihao,Chen Yiyu,Yuan Dong,Wen Tao,Ge Mingjian,Yu Qiubo
In this paper, we first synthesis three-dimensional jasmine-like Cu@L-aspartic acid(L-ASP) inorganic–organic hybrid nanoflowers to load palladium-platinum nanoparticles (Pd–Pt NPs) as the signal enhancer in order to quantify intracellular speckle-type POZ domain protein. Scanning electron microscope, fourier transform infrared, energy dispersive spectrometer, X-ray photoelectron spectroscopy analysis was used to characterize the newly synthesized materials. The newly formed Cu@L-Asp/Pd-PtNPs can catalyze the decomposition of hydrogen peroxide and exhibit excellent catalytic performance. When different concentration of speckle-type POZ domain protein is captured by speckle-type POZ domain protein antibody linked to the surface of Cu@L-Asp/Pd–Pt NPs, the current signal decreases with the increase concentration of speckle-type POZ domain protein. After optimization, the speckle-type POZ domain protein immunosensor exhibited a good linear response over a concentration range from 0.1–1 ng mL −1 with a low detection limit of 19 fg mL −1 . The proposed sensor demonstrates good stability within 28 days, acceptable reproducibility (RSD = 0.52%) and selectivity to the speckle-type POZ domain protein in the presence of possible interfering substances and has potential application for detecting other intracellular macromolecular substances.
研究领域:
分析化学
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生物化学
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纳米技术
·
生物传感器
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