ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Wentao Ding,Hao Li,Rui Zong,Jingyun Jiang,Xingfei Tang
The substitution of green hydrogen donors for replacing high-pressure H2 to achieve biomass derived ketone and aldehyde hydrodeoxygenation (HDO) under mild conditions has attracted widespread attention. However, it remains a considerable challenge to get rid of acid additives and control product selectivity. Herein, a series of bimetallic Pd–M/HZSM-5 catalysts (M = Zr, Mn, Zn, or La) were fabricated for controlled hydrodeoxygenation of biobased ketones and aldehydes (acetophenone, benzophenone, 4-hydroxyacetophenone, vanillin, furfural) using polymethylhydrosiloxane (PMHS) as the green H-donor, in which >99% conversion and >99% selectivity to ethylbenzene were achieved for hydrodeoxygenation of acetophenone as the probe within 3 h at 35 °C over the as-prepared 0.5%Pd–2.0%Zr/HZSM-5 catalyst with a Pd/Zr mass ratio of 1:4. According to characterizations of TEM-HAADF, XPS, ESR, and H2-TPR, the Pd–Zr alloy structure was formed on the bimetallic Pd–Zr/HZSM-5 catalyst, promoting the transform of Pd–O–Zr solid solution to PdO–ZrO2 and the generation of oxygen vacancy. Moreover, the abundant of oxygen vacancies on the alloyed Pd–Zr/HZSM-5 catalysts enhance the dissociation of silanes to provide the abundance of hydrogen protons, greatly accelerating the hydrogenation of biobased ketones and aldehydes, and then the acid site of the Pd–Zr/HZSM-5 catalyst promotes the dehydration of the intermediates (alcohols) to hydrocarbons. Furthermore, the as-fabricated Pd–Zr/HZSM-5 alloy catalyst can achieve an excellent recycling capability after six uses and exhibits universality toward various biobased ketones and aldehydes at 35 °C. The present findings provide new insights into the design of selective HDO of biomass in a green process.
研究领域:
催化
·
生物质转化
·
绿色化学
·
可持续能源
·
材料科学
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DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·Vol. 13
·期 12
·12226-12237
·
IF 1.5
Yanrong Li,Yao Liu,Zhongbin Li,Jiaqiang Li,Chaozhong Guo,Jin Zhang,Jinbiao Wang
Graphdiyne (GDY) as a novel allotrope has been theoretically predicted to be the most stable non-natural carbon allotropes. However, GDY has not been systematically investigated as a new carbon support to ORR catalysts. Thus, here we report a new strategy for the synthesis of Pd nanoparticles anchored on nitrogen-doped graphdiyne (CN x -Pd@GDY) electrocatalyst for oxygen reduction reaction (ORR) via a facile pyrolysis method. The results show that the prepared CN x -Pd@GDY catalyst has exhibited excellent ORR catalysis performance with a four-electron transfer pathway in 0.1 mol l -1 KOH electrolyte compared to other commercial carbon supports such as carbon black and carbon nanotubes. Electrochemical research results show that the as-formed CN x -Pd@GDY exhibits excellent electrocatalytic ORR activity with an onset potential of 0.96 V vs. RHE and a high long-term stability in the alkaline condition. The interaction between Pd nanocrystals and the encapsulating PANI shells was found in the catalyst, which markedly contributes to the improvement in ORR catalytic activity and stability of the catalyst. Such catalytic characteristics have reasonably indicated a great potential as a novel catalyst for ORR instead of the commercial Pt-based catalyst.
研究领域:
材料科学
·
电化学
·
纳米催化
·
能源材料
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DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·Vol. 12
·期 6
·5511-5520
·
IF 1.5
Xingpu Qi,Jianzhong Qian,Tong Chen,Daoli Lu,Bin Chen
With a chemical and eco-friendly in situ reduction technique, an excellent Ag-Pd bimetallic nanoparticle (Ag-Pd)-based hybrid was successfully synthesized in this study. To determine copper(II) ions in water, this work employed differential pulse adsorptive stripping voltammetry (DPAdSV) and preconcentration methods. Furthermore, the sensor feasibility was studied with river and tap water as real specimens. The results revealed the potential of the proposed electrochemical sensor to be applied for the early testing of water quality based on its desirable behavior in Cu(II) determination in real specimens.
研究领域:
环境化学
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电分析化学
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水质监测
·
纳米材料
·
传感器与生物传感器
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DOI
高影响因子
Scientific Reports
·
2017
·Vol. 7
·期 1
·7448
·
IF 4.259
Han Lina,Li Qinglian,Chen Shuai,Xie Wei,Bao Weiren,Chang Liping,Wang Jiancheng
A sort of magnetical material named Fe 3 O 4 –NH 2 –Pd was prepared by loading varying amounts of immobilizing Pd on the surface of the magnetic Fe 3 O 4 –NH 2 microspheres. This magnetical material was used firstly for capturing Hg° from coal derived fuel gas based on its recoverability. The experimental results showed that the loading Pd on the amine-functionalized magnetite nanoparticles can greatly improve the efficiency of removing Hg° at a high temperature range between 200 and 300 °C. The magnetic Fe 3 O 4 –NH 2 –Pd sorbent with 5% Pd loaded exhibited significantly high activity and stability in capturing Hg°, affording over 93% capture efficiency at 200 °C for more than 8 hrs. Compared to the Fe 3 O 4 –NH 2 sorbent that converted the Hg° as HgS, this Fe 3 O 4 –NH 2 –Pd sorbent can remove the Hg° by forming Pd-Hg amalgam and HgS. In addition, the experimental tests indicated that the as-synthesized Fe 3 O 4 –NH 2 –Pd sorbent still showed stable magnetic properties after two regeneration cycles in removing Hg°, which provided the opportunity for preparing a recyclable sorbent which can be easily separated and recovered for Hg° removal.
研究领域:
环境科学
·
材料化学
·
能源工程
·
污染控制
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Chuanxia Chen,Wendong Liu,Pengjuan Ni,Yuanyuan Jiang,Chenghui Zhang,Bo Wang,Jinkai Li,Bingqiang Cao,Yizhong Lu,Wei Chen
Enzyme-like activity and efficiency of nanomaterials are strongly controlled by their size, composition, and structure, and hence the structural parameters need to be optimized. Here, we report that two-dimensional Pd nanoplates enclosed by {100}-facets [{100}PdSP@rGO] exhibit substantially enhanced intrinsic oxidase-like activities relative to the {111}-facets ones and Pd nanocubes in catalyzing the chromogenic reaction of 3,3′,5,5′-tetramethylbenzidine. By taking ascorbic acid 2-phosphate as the substrate, which transforms to ascorbic acid in the presence of acid phosphatase (ACP), the {100}PdSP@rGO could be used as an efficient nanozyme for colorimetric ACP detection without resorting to destructive H2O2. A good linear relationship from 0.01 to 6.0 mU/mL with a detection limit of 8.3 μU/mL is obtained, which is better than most previously reported ACP assays. Importantly, the excellent assay performance could be successfully applied to ACP determination in serum samples with high accuracy. This study demonstrates that the enzyme-like activity of nanomaterials could be finely tuned simultaneously by controlling their exposed crystal facets and high specific surface area.
研究领域:
纳米酶学
·
生物分析化学
·
分子诊断
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纳米材料学
·
临床检验医学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 46
·23230-23239
·
IF 7.443
Chenhao Du,Yun Guo,Yanglong Guo,Xue-qing Gong,Guanzhong Lu
Developing methods for the fabrication of active and thermally stable noble metal/metal oxide nanomaterials are very important for catalysis and material fields. Herein, we used a polymer-template synthesis approach to prepare hollow Pd–CeO2 nanocomposite spheres (NCSs) with Pd nanoparticles evenly distributed inside the CeO2 shell, in which the aggregation of Pd nanoparticles can be well inhibited with the help of the protection of CeO2 nanocrystallites even after being calcined at 700 °C. The Pd nanoparticles are partially buried in the CeO2 shell and the surface Pd species are highly ionic, which is caused by the electron exchange at the Pd–CeO2 interface during calcination. This hollow structure Pd–CeO2 nanocatalyst shows excellent catalytic activity and stability in the aqueous selective reduction of 4-nitrophenol and gaseous CO oxidation. For the selective reduction of 4-nitrophenol, the reaction rate of this h-Pd–CeO2 NCS catalyst compared to those of the supported Pd/CeO2 and physically mixed Pd + CeO2 catalysts is almost 14 times and 5 times faster, respectively. For the CO oxidation, the larger Pd–CeO2 interface in h-Pd–CeO2 NCSs could facilitate the reaction between the adsorbed CO and O2, thus showing better low temperature activity. This paper emphasizes the advantages of a core–shell hollow structure and provides a new way for obtaining novel functional nanocatalysts.
研究领域:
材料化学
·
纳米催化
·
无机功能材料
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环境催化
·
能源材料
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DOI
高影响因子
Theranostics
·
2026
·Vol. 16
·期 13
·7571
·
IF 14.9
Linlin Song,Meixu Chen,Huiling Wang,Xin Wang,Tianyue Xu,Heqing Zhang,Shuwen Ran,Liwen Huang,Yingying Ma,Zhihui Liu,Zihan Xu,Yujie Zhao,Zichang Liu,Yong Luo,Xiujun Yu,Yulan Peng,Hubing Shi,Jing Jing,Xiujing He
Rationale Triple-negative breast cancer (TNBC) remains one of the most aggressive subtypes due to its poor immunogenicity and resistance to systemic therapies. Methods Here, we report a multifunctional NIR-II light-triggered theranostic nanoplatform, termed LQPO, that integrates liposome, Ti 3 C 2 quantum dots (QDs), perfluorohexane (PFH), and ozone to enable multimodal imaging-guided photo-gas synergistic therapy. The QDs, embedded within the liposomal bilayer, act as highly efficient NIR-II photothermal transducers, while the PFH core serves as a liquid-gas phase-change medium capable of dissolving and releasing ozone under localized heating. Results Upon NIR-II irradiation, LQPO produced strong photothermal and photoacoustic signals for real-time photoacoustic (PA) and contrast-enhanced ultrasound (CEUS) imaging, accompanied by vaporization of the PFH core and burst release of ozone. This spatiotemporally coordinated cascade induced potent oxidative stress and hyperthermia, synergistically driving GSDME-dependent pyroptosis and immunogenic cell death (ICD). The resulting “in situ vaccination” effect remodeled the tumor immune microenvironment and primed tumors for PD-1 blockade therapy. In vivo , NIR-II-activated LQPO achieved efficient tumor accumulation, strong PA/CEUS imaging contrast, and pronounced inhibition of both primary and abscopal tumors when combined with αPD-1 therapy. No significant systemic toxicity was observed, confirming its favorable biosafety. Conclusions Overall, this study establishes a single-laser-activated nanoplatform that unifies real-time multimodal imaging and photo-gas synergistic therapy, and converts localized treatment into a systemic antitumor immune response upon integration with checkpoint inhibition.
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DOI
PubMed
高影响因子
ACS Sensors
·
2026
·
IF 10.9
Xinxin He,Ping Guo,Yinhua Hu,Xuyang An,Shuai Liang,Tiezhu Liu,Tong Zhang,Guohua Cai,Yanjie Chu,Jia Zhang
Exhaled human breath contains disease-related biomarkers, enabling non-invasive medical diagnostics. Small intestinal bacterial overgrowth (SIBO) is traditionally diagnosed through hydrogen measurement, a method that offers limited specificity and sensitivity. Herein, we introduce a simplified Pt/Pd-SnO2 electronic composed of using only two sensing materials to achieve multi-gas detection. By simultaneously monitoring H2, CO, ethanol, and acetone, the system provides a more informative diagnostic profile than conventional single-marker tests. Furthermore, the electronic nose employs dual operating temperatures (135 and 190 °C) to enhance gas discrimination. Machine learning-assisted signal processing further optimizes the system’s ability to differentiate gases, enabling more accurate detection in clinical settings. It achieves a 93% classification accuracy and a mean squared error of 0.78 for gas concentration estimation. Importantly, the system was validated using real clinical breath samples collected after lactulose ingestion, where SIBO patients exhibited markedly elevated responses (7.62−18.77) compared to healthy individuals (2.45−4.91). This clinically validated, multi-gas platform offers improved accuracy and practical potential for SIBO diagnosis.
✓ 已验证
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·Vol. 41
·期 2
·944-950
·
IF 3.313
Ning-Zhao Shang,Cheng Feng,Shu-Tao Gao,Chun Wang
In this study, a bi-metal based nanocatalyst (AgPd@UIO-66-NH 2 ) was synthesized by immobilizing AgPd nanoparticles onto the amino-functionalized metal-organic framework material (UIO-66-NH 2 ). The catalytic activity of AgPd@UIO-66-NH 2 for the hydrolysis of ammonia borane was evaluated. Among all the prepared AgPd@UIO-66-NH 2 catalysts, the Ag 1 Pd 4 @UIO-66-NH 2 exhibited the highest catalytic activity for the hydrolysis of ammonia borane with a turnover frequency value of 90 mol H 2 mol catalyst −1 min −1 , which is among the higher value of the previous reports.
研究领域:
材料科学
·
催化化学
·
纳米技术
·
氢能
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2014
·
IF 5.211
Yan Tong,Xiaofeng Lu,Weining Sun,Guangdi Nie,Liu Yang,Ce Wang
A high-performance hydrogen generation system based on the electrospun polyacrylonitrile (PAN)/Ag/Pd composite nanofibers , which were prepared by microwave reducing the electrospun PAN/AgNO 3 nanofibers and followed by a replacement reaction has been demonstrated. The morphology of the as-prepared PAN/Ag/Pd composite nanofibers and the metal nanoparticles on the fibers were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), high resolution TEM (HRTEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) measurements. It has been demonstrated that the obtained PAN/Ag/Pd composite nanofibers possess fine morphology and high catalytic activities for H 2 generation from aqueous solution of ammonia borane (NH 3 BH 3 , AB). The H 2 generation test exhibited that the catalyst had excellent catalytic activity (with turnover frequency (TOF) of 377.2 mol H 2 h −1 (mol Pd) −1 ), good recycle stability and easy-separation from the reaction system. This new kind of nanofibers possesses great potential application for the new clean energy development.
研究领域:
材料科学
·
催化化学
·
氢能
·
纳米技术
·
能量转换
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Ziling Zhang,Junhao Ma,Yu Deng,Yuan Ren,Wenhe Xie,Yonghui Deng,Yidong Zou,Wei Luo
Hydrogen as an important clean energy source with a high energy density has attracted extensive attention in fuel cell vehicles and industrial production. However, considering its flammable and explosive property, gas sensors are desperately desired to efficiently monitor H2 concentration in practical applications. Herein, a facile polymerization-induced aggregation strategy was proposed to synthesize uniform Si-doped mesoporous WO3 (Si-mWO3) microspheres with tunable sizes. The polymerization of the melamine–formaldehyde resin prepolymer (MF prepolymer) in the presence of silicotungstic acid hydrate (abbreviated as H4SiW) leads to uniform MF/H4SiW hybrid microspheres, which can be converted into Si-mWO3 microspheres through a simple thermal decomposition treatment process. In addition, benefiting from the pore confinement effect, monodispersed Pd-decorated Si-mWO3 microspheres (Pd/Si-mWO3) were subsequently synthesized and applied as sensitive materials for the sensing and detection of hydrogen. Owing to the oxygen spillover effect of Pd nanoparticles, Pd/Si-mWO3 enables adsorption of more oxygen anions than pure mWO3. These Pd nanoparticles dispersed on the surface of Si-mWO3 accelerated the dissociation of hydrogen and promoted charge transfer between Pd nanoparticles and WO3 crystal particles, which enhanced the sensing sensitivity toward H2. As a result, the gas sensor based on Pd/Si-mWO3 microspheres exhibited excellent selectivity and sensitivity (Rair/Rgas = 33.5) to 50 ppm H2 at a relatively low operating temperature (210 °C), which was 30 times higher than that of the pure Si-mWO3 sensor. To develop intelligent sensors, a portable sensor module based on Pd/Si-mWO3 in combination with wireless Bluetooth connection was designed, which achieved real-time monitoring of H2 concentration, opening up the possibility for use as intelligent H2 sensors.
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 18
·8785-8796
·
IF 3.3
Jiaxin Zhang,Xianlang Chen,Jinhua Yu,Zheng Fang,Lele Yan,Zijian Wang,Zhengyu Pan,Rongrong Li,Li Zhang
Catalytic hydrodechlorination (HDC) is considered as one of the most promising strategies for the treatment of chlorinated environmental pollutants. Here we proposed a strategy for rapid complete dechlorination by exploiting a B–N co-doped hierarchically porous carbon material (BNC) to immobilize Pd NPs, which makes use of not only the micro/meso porous structure to accelerate the mass transport and to provide enormous active sites, but also the synergistic effect for codoping of B–N to enhance the interaction between Pd NPs and support and thus to stabilize and disperse the small size of the Pd particle. Ascribed to these combined advantages, Pd/BNC exhibited more distinctive catalytic dehalogenation activity (k = −0.14 min−1) and better stability (about 90.0% activity retention after 5 cycles) than Pd/C (k = −0.0070 min−1). Additionally, density functional theory (DFT) calculation indicates that the incorporation of N and B atoms in the carbon skeleton will reduce the adsorption energy of Cl− and thus Pd/BNC exhibits more remarkable stability than Pd/C during long-term HDC reactions. As a result, ultrafine Pd particles and high Pd2+/(Pd2+ + Pd0) ratios were found in Pd/BNC.
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产品关联
DOI
高影响因子
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