SENSORS AND ACTUATORS B-CHEMICAL
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2020
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IF 7.1
Boxuan Yang,Zheng Zhang,Chen Tian,Wenjing Yuan,Zhongqiu Hua,Shurui Fan,Yi Wu,Xuemin Tian
Gas sensors based on Pd-loaded SnO 2 were prepared with printed zeolite films on the top of the sensor layer to enhance selective response to methane. As expected, Pd-loaded SnO 2 has a sensitive response to CH 4 and VOCs, such as ethanol and acetone vapors. Pt catalyst was dispersed onto the surface to promote the catalytic activity of zeolite. According to the catalytic characterizations, it was indicated that interfered gases, CO and ethanol were catalytically oxidized into CO 2 and water vapor. Whereas the catalytic combustion of methane is a negligible and sensitive response to the interested analyte was significantly promoted. Thus, the selective response to CH 4 was greatly improved even in a mixture of CO and VOCs. Based on the power-law response to oxygen, it was found that the resistive responses of all sensors were highly oxygen-dependent, suggesting that oxygen adsorbates on the surface were involved in the sensing process and no difference with zeolite coated sensors. Thus, it can be concluded that zeolite films printed onto the sensing layer surface serve as a catalytic filter and responsible for the enhanced sensitive and selective response of methane.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
ACS ES&T Engineering
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2024
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IF 7.4
Lan-Ying Liu,Min-Hua Cui,Shi-Ming Niu,Xue-Dong Zhang,Xin-Hui Li,Wo-Long Wang,He Liu,Guo-Shuai Liu,Ai-Jie Wang
In this study, we synthesized a phosphorus-coordinated Pd@MXene catalyst to address the drawbacks associated with high noble metal usage, susceptibility to poisoning, and stability issues in the electrocatalytic hydrodehalogenation (EHDC) of recalcitrant halogenated pollutants. The phosphorus-coordinated Pd@MXene exhibited an EHDC performance comparable to that of the benchmark electrode (Pd@MX/CC) when tested on the model pollutant diclofenac (DCF). Notably, the phosphorus-coordinated Pd electrode demonstrated an 80% reduction in Pd usage and a 3.9-fold increase in Pd utilization efficiency. This improved performance was consistent across a wide range of pH values (pH 3, 7, and 11) and was sustained over 10 reaction cycles for the removal of DCF. Furthermore, the enhanced catalytic activity of the phosphorus-coordinated Pd electrode was achieved in the EHDC of various halogenated compounds. Importantly, the electrode exhibited a favorable tolerance to inorganic ions during the EHDC process. Density functional theory (DFT) calculations provided insights into the electronic configuration regulation of phosphorus-coordinated Pd@MXene, optimizing binding energies for H* and dechlorinated intermediates. The reported promotion effect of halogenated pollutants degradation by the phosphorus-coordination approach offers new insights into efficient EHDC systems toward water purification.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
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2021
·Vol. 68
·期 10
·1897-1907
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IF 1.967
Zhen Zhu,Yu-Teng Hwang,Hao-Chun Liang,Ren-Jang Wu
In this study, several Pd/MgO/BiVO 4 nanocomposites were prepared using the hydrothermal method and their effective photocatalyst activity for the photoreduction of CO 2 to CH 4 was investigated. The microstructure and photocatalytic behavior of the prepared photocatalysts were studied through X-ray diffraction, scanning electron microscopy, tunneling electron microscopy, X-ray photoelectron spectroscopy, ultraviolet–visible spectrophotometry, Fourier-transform infrared spectroscopy, Brunauer–Emmett–Teller specific surface area, and photoluminescence spectroscopy. CH 4 yields of 5.9 and 9.4 μmol g −1 hr −1 were obtained using BiVO 4 and 25% MgO/BiVO 4 nanocomposites, respectively. The highest production rate of CH 4 was measured as 12.8 μmol g −1 hr −1 on overloading 0.3% Pd on 25% MgO/BiVO 4 . Pd/MgO/BiVO 4 exhibited excellent CO 2 photoreduction stability with negligible loss after five consecutive cycles. Finally, a possible mechanism of CO 2 photoreduction using Pd/MgO/BiVO 4 was proposed for understanding the synergistic effects. The results of the experiment revealed that Pd/MgO/BiVO 4 can be a promising photocatalyst in solar energy conversion and storage application and can achieve excellent CO 2 photoreduction performance.
研究领域:
材料科学
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环境科学
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能源科学
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2021
·Vol. 31
·期 51
·2107181
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IF 18.808
Wen Zhang,Xue Jiang,Zemeng Dong,Jing Wang,Ning Zhang,Jie Liu,Guang-Rui Xu,Lei Wang
Modulating the morphology and chemical composition is an efficient strategy to enhance the catalytic activity for water splitting, since it is still a great challenge to develop a bifunctional catalyst for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) over a wide pH range. Herein, Pd/NiFeO x nanosheets are synthesized with tightly arranged petal nanosheets and uniform mesoporous structure on nickel foam (NF). The porous 2D structure yields a larger surface area and exposes more active sites, facilitating water splitting at all pH values. The overpotential of Pd/NiFeO x nanosheets for OER is only 180, 169, and 310 mV in 1 m KOH, 0.5 m H 2 SO 4 , and 1 m phosphate-buffered saline (PBS) conditions at 10 mA cm −2 current density, as well as excellent HER activity with ultralow overpotential in a wide pH range. When using porous Pd/NiFeO x nanosheets as bifunctional catalysts for water splitting, it just required a cell voltage of 1.57 V to reach a current density of 20 mA cm −2 with nearly 100% faradic efficiency in alkaline conditions, which is much lower than that of benchmark Pt/CǁRuO 2 (1.76 V) couples, along with the improving stability benefiting from the good corrosion resistance of the inner NiFeO x nanosheets.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Huizhen Sun,Xiuhua Chen,Shaoyuan Li,Wenhui Ma,Xiumin Chen,Dandan Wu,Kaixin Fu,Mingjun Xiao,Ming Wen
Developing efficient and selective recovery of Pd(II) adsorbents is crucial for addressing environmental pollution issues. Among them, covalent organic framework (COF) and metal organic framework (MOF) composites due to the multi-site functional groups are expected to exhibit excellent Pd(II) adsorption. However, the design and preparation of COF and MOF composite adsorbents for highly efficient adsorption of heavy metal Pd(II) still face many challenges. Herein, we constructed a series of novel core–shell structure UiO-66-NH 2 @TAP-COF (denoted as M@C) adsorbents (M@C-X, X = 1–5, representing different MOF doses) by Schiff base reaction and applied in the adsorption of Pd(II). The findings indicated that the M@C-3 exhibited ultra-high adsorption performance, reaching a capacity of 2134.1 mg/g, and displayed excellent selectivity, making it the best among similar materials. Experimental data and density functional theory (DFT) calculations revealed that the efficient and selective adsorption of Pd(II) is attributed to coordination interaction and strong electrostatic between Pd(II) and the abundant N and O groups in M@C. This work demonstrates the significant potential of the constructed core–shell M@C composites for the efficient and selective recovery of precious metal Pd(II).
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
TOPICS IN CATALYSIS
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2024
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IF 2.8
Wang Xinyu,Xu Xin,Xiong Wuwan,Ye Daiqi,Chen Peirong
Catalytic oxidation is an effective solution for the control of methane (CH 4 ) emission in exhausts from natural gas vehicles. Pd-based small-pore zeolites (such as Pd-SSZ-13) are considered to be the most active catalysts for CH 4 oxidation, but H 2 O in the exhausts tends to induce deactivation of Pd catalysts. In this work, we tuned the hydrophobicity of Pd-SSZ-13 as a representative to improve its H 2 O resistance in CH 4 oxidation. Pd-SSZ-13 catalysts with different Si/Al ratios were obtained by dealuminizing the pristine SSZ-13 zeolite with acid followed by Pd ion exchange, and a reduction of T 50 (i.e. the temperature to reach 50% conversion of CH 4 ) by 20 ℃ was achieved in CH 4 oxidation in the presence of 10 vol.% H 2 O. Detailed physicochemical characterizations showed that the fraction of highly dispersed PdO species (highly active in CH 4 oxidation) increased, whereas that of less inactive PdO x clusters decreased, in the Pd-SSZ-13 after acid modification. In addition, the increase of zeolite hydrophobicity after acid modification alleviated the H 2 O inhibition effect on the active PdO phase, leading to a less activity loss of Pd-SSZ-13 in CH 4 oxidation. The improved hydrophobicity also favored C 3 H 8 combustion over Pd-SSZ-13. These results suggested that simple acid modification could tune effectively the Si/Al ratio and hydrophobicity of zeolite supports, and eventually the physicochemical properties and oxidation performance of the supported Pd catalysts.
研究领域:
催化化学
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环境科学
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DOI
高影响因子
MOLECULES
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2022
·Vol. 27
·期 5
·1482
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IF 4.927
Yacong An,Xundou Li,Fengjiao Yao,Jinhong Duan,Xian-Da Yang
The PD-1/PD-L1 pathway blockade can generate a good clinical response by reducing immunosuppression and provoking durable antitumor immunity. In addition to antibodies, aptamers can also block the interaction between PD-1 and PD-L1. For the in vivo application, however, free aptamers are usually too small in size and quickly removed from blood via glomerular filtration. To avoid renal clearance of aptamer, we conjugated the PD-L1 aptamer to albumin to form a larger complex (BSA-Apt) and evaluated whether BSA-Apt would enhance the in vivo antitumor efficacy. The PD-L1 aptamer was thiol-modified and conjugated to the amino group of BSA via a SMCC linker. The average size of BSA-Apt was 11.65 nm, which was above the threshold for renal clearance. Functionally, BSA-Apt retained the capability of the PD-L1 aptamer to bind with PDL1-expressing tumor cells. Moreover, both the free aptamer and BSA-Apt augmented the PBMC-induced antitumor cytotoxicity in vitro. Furthermore, BSA-Apt generated a significantly stronger antitumor efficacy than the free PD-L1 aptamer in vivo without raising systemic toxicity. The results indicate that conjugating the PD-L1 aptamer to albumin may serve as a promising strategy to improve the in vivo functionality of the aptamer and that BSA-Apt may have application potential in cancer immunotherapy.Keywords:PD-L1;aptamer;albumin;BSA-Apt;cancer;immunotherapy
研究领域:
肿瘤学
·
免疫学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2020
·
IF 2.369
Yongkang Lu,Bo Zhang,Shaobo Liu,Luxia Yin,Wanghui Gong,Jianguang Gao,Zekai Zhang,Wensheng Ning
Pd/SiO2-n aerogel composites with different Si/Pd mole ratios (n(Si/Pd)) were synthesized by a sol–gel method followed by drying in the atmosphere to adsorb thiophenic compounds from model oils. For Pd/SiO2-n, doping Pd species in SiO2 aerogels led to the appearance of weak Lewis acidic sites on the surface. The adsorption capacity of Pd/SiO2-n was significantly higher than that of pure SiO2, owing to the π-complexation, S–M bonding, and acid–base interaction between Pd2+ and thiophenic compounds. Among them, the capacity of Pd/SiO2-318 was the highest, 4.76 mg S/gads (i.e., 9.37 μmol S/μmol Pd), which was obviously higher than that of sorbents reported such as Pd/activated carbon and Pd/Al2O3, based on the amount of thiophene adsorbed per unit active centers. In the presence of aromatics and olefins, the selectivity of Pd/SiO2 for thiophene was higher than that of Ag/SiO2 and Cu/SiO2 reported, attributed to the stronger S–Pd bonding than the S–Ag and S–Cu bonding. The equilibrium adsorption data of thiophene onto Pd/SiO2-318 were well simulated with the Langmuir and Freundlich models. Combined with thermodynamic results, it can be found that the low temperature was favorable for the adsorption of thiophene. Pd/SiO2 exhibited a good regeneration performance after solvent washing.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Xiulan Weng,Huijing Ma,Gary Owens,Zuliang Chen
Recently, bimetallic Fe-Pd nanoparticles were integrated with metal organic frameworks (MOFs) to produce a new composite catalyst with significant potential for organic contaminant removal due to enhanced adsorption and reduction. Here, 85.9 % of 2,4-dichlorophenol (2,4-DCP) was successfully removed from aqueous solution within 120 min when using a zinc-based zeolitic imidazolate framework (ZIF-8) embedded with Fe-Pd (Fe-Pd@ZIF-8). In comparison only 77.4 and 48.3 % was removed when using ZIF-8 or Fe-Pd alone. Thus, to better understand the function of composite components (ZIF-8 and Fe-Pd) in the removal of 2,4-DCP, and the specific removal mechanism involved, Fe-Pd@ZIF-8 was characterized before and after exposure to 2,4-DCP. This comparison revealed that 2,4-DCP was adsorbed onto the surface of the composite during exposure. Moreover, while ZIF-8 maintained stability following the removal of 2,4-DCP, Fe 0 was partially oxidized and Pd functioned as a catalyst in the removal process. Furthermore, kinetic studies demonstrated that the initial adsorption of 2,4-DCP conformed to a pseudo-second-order model and the subsequent reduction conformed to a pseudo-first-order model, whereas isothermal adsorption best fit the Freundlich adsorption model. This observation suggested that removal mechanism of 2,4-DCP involved both adsorption and dechlorination. Finally, Fe-Pd@ZIF-8 was applied to practically remove 2,4-DCP from wastewater, showing a 74.4 % removal efficiency which indicated that the composite was a potential new nanomaterial for practically removing organic contaminants from wastewater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Xiaosong Zhou,Xiaoxing Yu,Lanzhen Peng,Jin Luo,Xiaomei Ning,Xuliang Fan,Xunfu Zhou,Xiaoqin Zhou
The photocatalytic H 2 production activity of polymer carbon nitride (g-C 3 N 4 ) is limited by the rapid recombination of photoelectron-hole pairs and slow surface reduction dynamic process. Here, a supramolecular complex (named R-TAP-Pd(II)) was fabricated via self-assembly of (R)-N-(1-phenylethyl)-4-(4-(pyridin-2-yl)-1H-1,2,3-triazol-1-yl)benzamide (R-TAP) with Pd(II) and used to modify g-C 3 N 4 . In the R-TAP-Pd(II)@g-C 3 N 4 composite photocatalyst, the spin polarization of R-TAP-Pd(II) can promote charge transfer and inhibit photogenerated carrier recombination, as confirmed by spectral tests and photoelectrochemical performance tests. Electrochemical tests and in situ X-ray photoelectron spectroscopy (XPS) tests proved that the Pd(II) ion in the R-TAP-Pd(II) molecule can serve as active sites to accelerate H 2 production. The R-TAP-Pd(II)@g-C 3 N 4 presented a photocatalytic H 2 generation rate of 1085 μmol g −1 h −1 when exposed to visible light, which was a about 278-fold increase compared with g-C 3 N 4 . This work finds a new approach to boost the photocatalytic efficiency of g-C 3 N 4 via supramolecular self-assembly.
研究领域:
材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Yinghua Xu,Tingjie Ge,Hongxing Ma,Xufen Ding,Xiaoyong Zhang,Qi Liu
Hydrodefluorination (HDF) is the key step in fluoroaromatic pollutant (FAP) degradation, making the search for efficient HDF catalysts and the determination of the corresponding mechanism a matter of great importance. In this study, we developed an efficient HDF catalyst (a Rh-Pd alloy) and investigated the underlying catalytic reaction mechanism , using 4-fluorophenol (4-FP) as a model FAP. Specifically, the rapid aqueous-phase HDF of 4-FP at pH 3 was achieved on a Rh-Pd alloy-modified Ni foam electrode, which was followed by ring hydrogenation (RH) of the HDF product (phenol) to afford cyclohexanone and cyclohexanol . Inductively coupled plasma optical emission spectrometer (ICP-OES) and thermodynamic analyses showed that, in addition to those supplied by the applied current, the electrons involved in the HDF of 4-FP and the RH of phenol were largely provided by the oxidative dissolution of the Ni foam support. Hydrogenation and cyclic voltammetry experiments indicated that the HDF of 4-FP probably follows an indirect mechanism (featuring adsorbed H atoms as the direct reductant) and that the strength of 4-FP adsorption onto the surface of the catalyst significantly influences its HDF activity.
研究领域:
环境科学
·
电化学
·
催化材料
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产品关联
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Zhe Zhang,Jianan Zhang,Shuai Chen,Yanan Liu,Yufei He,Dianqing Li
Hydrogen spillover phenomenon can significantly impact the activity in hydrogenation reaction, but the spillover is limited in a very short range on non-reducible Al 2 O 3 , a most widely used industrial support. Herein, Al 2 O 3 doped with different lanthanides (ln) was prepared by co-precipitation, which was then used to produce Pd/ln-Al 2 O 3 catalysts. These catalysts display much higher hydrogenation activity towards alkylated anthraquinone than undoped Pd/Al 2 O 3 catalyst and those modified by non-lanthanide elements. After the introduction of lanthanides, the reaction order of H 2 decreases from 1 to 0. Further characterization and DFT calculation show that H 2 storage ability is increased for ln-doped catalysts due to the low activation energy of H transfer and low adsorption energy of H on O(-ln) sites. In addition, a reasonable relationship between reducibility of ln 3+ in catalysts and the catalytic performance is found.
研究领域:
化学工程
·
催化科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）