ACS Applied Energy Materials
·
2022
·
IF 6.959
De Ping Chen,Lei Yuan,Meng Jue Li,Wen Jing Han,Xu Dong Liu,Xi Chuan Liu,Chao Yang Wang
Pd is a highly active non-Pt anode in direct ethanol fuel cells, and its morphology and structural composition heavily influence its electrocatalytic efficiency. In this study, three-dimensional (3D)-hollow Au microspheres (HNPs-Au) as a support for the Pd monolayer (HNPs-Au@Pd) were synthesized using a simple template method and galvanic replacement reaction. The experimental results and theoretical calculations show that the presence of HNPs-Au enhances the catalytic activity of ethanol oxidation in alkaline media, improving the electroactivity of metallic Pd. Benefiting from the 3D-hollow-porous structure and the significant synergistic impact between Au and Pd (balancing the adsorption energy of the intermediate and reactant molecules), HNPs-Au@Pd achieves a 10.8-fold mass activity and a 3.3-fold enhancement of the specific activity for the ethanol oxidation reaction when compared to commercial Pd/C. The present work not only enriches the preparation strategy of porous metal materials but also opens up a sector for the construction of anodic electrocatalysts with a wide range of applications.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8855-8862
·
IF 3.925
Yabing Tian,Chen Xing,Wenxiang Wang,Shiguo Zhang,Yan Zhang
Pd-catalyzed Suzuki–Miyaura cross-coupling reactions have attracted considerable attention. Porous organic polymers (POPs) are potential heterogeneous catalysts to overcome the shortcomings of the homogeneous reaction. However, most POPs are microporous, which strongly hindered the mass transfer process during the catalytic reaction. In this work, a Pd-containing, highly crosslinked, mesoporous poly(ionic liquid) (SMPIL–Pd) was designed as a heterogeneous catalyst for efficient Suzuki–Miyaura coupling reactions. This catalyst was fabricated by hyper-crosslinking of a salen-containing mesoporous poly(ionic liquid) via a simple Friedel–Crafts alkylation reaction followed by Pd(II) coordination via the –N2O2– tetradentate structure of the salen structure. A series of characterization studies revealed that SMPIL–Pd possesses predominant porosity and extremely rigid networks, highly dispersed catalytic active sites, mesoporous structures, and large specific surface areas. Consequently, this catalyst exhibited excellent catalytic activity towards Suzuki–Miyaura coupling reactions under an air atmosphere in 50% aqueous ethanol. SMPIL–Pd also demonstrated outstanding stability and recyclability, and it can be reused seven cycles without a significant loss of activity.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 11
·15337-15346
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IF 5.19
Yang Zhen-xing,Shang Jie,Yan Guang-xu,Wang Yu-xian,Guo Shao-hui
In this paper, Pd-Sn modified Ru-Ir electrode was prepared by thermal oxidation method, and the effects of doping amount of Pd-Sn and synthesis conditions on Pd-Sn modified Ru-Ir electrode performance were studied. Linear sweep voltammetry(LSV), cyclic voltammetry(CV), and the Tafel curve were used to study the electrochemical performance of the Pd-Sn modified Ru-Ir electrode materials. The effects of the doping amount of Pd-Sn on the microstructure and valence states of Pd-Sn modified Ru-Ir electrode materials were investigated by SEM, TEM, XRD, and XPS. When the mass of Pd-Sn accounted for 1.5% of the total mass of the elements, the molar ratio of Ru-Ir was 2:1, and the molar ratio of Pd-Sn was 3:1; the LSV, CV, and the Tafel curves indicated that Pd-Sn modified Ru-Ir electrode had the lowest chlorine evolution potential (1.0640 V vs. SCE), the best CV curve coincidence, and the smallest corrosion current density (6.5 × 10 −4 A/cm 2 ), showing the best chlorine evolution performance, the best durability, and corrosion resistance; the characterization of SEM, TEM, XRD, and XPS showed that Pd-Sn was successfully doped into Ru-Ir electrode materials; the crystallinity of Pd-Sn modified Ru-Ir electrode was the highest, and the binding energy was the lowest, but the crystal form of Ru-Ir solid solution did not have changed. The optimal synthesis conditions of Pd-Sn modified Ru-Ir electrode material were as follows: Pd-Sn molar ratio was 3:1, calcination temperature was 500 ℃, calcination time was 4 h, and water was used as solvent. Pd-Sn modified Ru-Ir electrode can efficiently treat high chlorine ammonia–nitrogen wastewater, when the reaction volume was 200 mL, the initial concentration of NH 3 -N was 100 mg/L, the concentration of chloride ion was 5000 mg/L, the current was 0.75 A, and the reaction time was 40 min; the removal rate of ammonia nitrogen can reach 100%. Responsible editor: Weiming Zhang.
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PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Xing Gao,Yingying Ding,Lilin Peng,Dan Yang,Xiaoyue Wan,Chunmei Zhou,Wen Liu,Yihu Dai,Yanhui Yang
Aqueous phase hydrogenative rearrangement of furfural (FAL) to cyclopentanone (CPO) via furfuryl alcohol (FOL) has been studied over Pd catalysts supported on H–ZSM–5 zeolites. Pd states, zeolite properties and reaction condition parameters were optimized, affording 98% selectivity and 120 h −1 specific reaction rate over 2% Pd/H–ZSM–5(25) catalyst at 160 °C and 3 MPa H 2 . For hydrogenation of FAL–to–FOL, the activity was related to the Si/Al ratio and acid property of zeolite supports. For hydrogenative rearrangement of FOL–to–CPO, pure H–ZSM–5 zeolite could catalyze single–step conversion with relatively low reaction rate, whereas the presence of Pd sites could achieve multi–step transformation with remarkably increased rate, highlighting Pd–zeolite acid sites synergy. Proton and furanylmethoxy–relevant intermediates were captured with spin trapping electron paramagnetic resonance experiments, and 4–hydroxy–2–cyclopentenone and 2–cyclopentenone were also identified as key intermediates in tandem reaction pathway to produce CPO.
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高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 152
·期 11
·3437-3446
·
IF 2.936
Yue Yihang,Li Yong,Wang Tingting,Wang Shifeng,Han Lin,Du Chun
A Pd/CeO 2 -M with high methanol oxidation performance was prepared from metal–organic framework (MOF). The reaction results indicate that the Pd/CeO 2 -M could achieve 100% methanol oxidation at 200 °C over the traditional Pd/CeO 2 -C at 350 °C. The high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), and Raman show that the Pd was uniformly distributed over the CeO 2 that was rich in oxygen vacancies. The methanol temperature program surface reaction (MeOH-TPSR) demonstrates that the Pd/CeO 2 -M could effectively decompose methanol at a lower temperature with the assistance of oxygen vacancies compared with Pd/CeO 2 -C. Methanol oxidation was conducted with in-situ Raman, CO diffuse reflectance infrared Fourier transformed spectroscopy (CO-DRIFTS) and in-situ DRIFTS to elucidate the reaction mechanism and establish the structure–activity relationship. The oxygen vacancies have participated in the assistance of methanol oxidation, which was revealed via in-situ Raman. The CO-DRIFTS indicates that the chemisorbed CO was more in linear form, which demonstrates that the Pd particles were over CeO 2 -M with a smaller size. The in-situ DRIFTS experiments show the methanol could be further effectively oxidized to bidentate formate over Pd/CeO 2 -M with the assistance of oxygen vacancies. The Pd/CeO 2 -M catalysis and its enhancement mechanism studies provided a potential strategy in the VOC removal catalysis development. Graphical Abstract
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Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 12
·2028-2037
·
IF 7.571
Chen Yang,Wenli Jiang,Yongqi Yu,Hui Zhang,Chenxin Cai,Qingming Shen
The integration of photothermal therapy (PTT) and photodynamic therapy (PDT) has become a promising cancer treatment method. Herein, anisotropic metal hetero-nanostructure Pd-tipped Au nanorods (PTA NRs) were fabricated, which exhibit plasmon-enhanced photothermal performance under near-infrared laser irradiation. Due to their anisotropic nanostructure, PTA NRs promote the generation of energetic hot electrons and prolong the separation time of electrons and holes. The hot electrons could generate heat energy through the electron–phonon relaxation process and produce reactive oxygen species through energy and electron transformation processes. Because of their high NIR absorption cross-section, as well as good photostability, PTA NRs can be used for NIR-activated photoacoustic imaging-guided PTT-PDT combination cancer therapy. Experiments in tumor-bearing mice proved that PTA NRs exhibit excellent anti-tumor effects, with little side effects on normal organs, making them promising for NIR cancer phototherapy.
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PubMed
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Siteng Rong,Hongzi Tan,Zhaobin Pang,Zhiyuan Zong,Rongrong Zhao,Zhihe Li,Zhe-Ning Chen,Ning-Ning Zhang,Weiming Yi,Hongyou Cui
Lignin could be depolymerized into large amount of phenolic compounds via fast pyrolysis . The upgrade of phenolic compounds via hydrodeoxygenation (HDO) involves multiple reaction pathways. It is challenging to selectively remove the oxygen-containing groups while keeping the aromatic rings intact. In this work, hierarchical Nb 2 O 5 (H–Nb 2 O 5 ) microspheres with abundant oxygen vacancies were synthesized to anchor the Pd clusters, which is featured with strong metal-support interaction via the electron transfer between Pd species and Nb species. For phenol HDO reaction, the oxygen vacancies were prone to interact with the phenolic hydroxy groups, resulting in phenol molecule adsorbed in a “nonplanar” manner, greatly weakening the C Ar -O bonds and averting the ring hydrogenation. Besides, the activated hydrogen atoms on Pd clusters could migrate to the vicinity of oxygen vacancies via spillover, promoting the cleavage of C Ar -O bond to obtain benzene. Current work provides a deep insight into the synergetic catalytic mechanism of Pd/H–Nb 2 O 5 catalyst for phenol HDO reaction, and also sheds light on the design and synthesis of high-efficient catalysts in other heterogeneous catalysis fields.
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高影响因子
FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Xin Zhang,Jingyun Jiang,Hao Li
Hydrodeoxygenation (HDO) of bio-oils obtained by rapid pyrolysis of biomass into high value-added chemicals generally required harsh conditions. Herein, three kinds of mixed-phase ZrO 2 supports (denoted as ZSX, X = 2–4) with different crystal structure proportions were prepared by one-pot hydrothermal synthesis method, and their performance on the properties of Pd/ZrO 2 catalysts were investigated for vanillin HDO. Pd/ZS3 exhibited excellent efficiency in HDO of vanillin, a typical model compound of lignin, achieving approximately 100% yield of 2-methoxy-4-methylphenol (MMP) in presence of n-butanol as solvent and polymethyl hydrogen siloxane (PMHS) as hydrogen donor under mild conditions (35 °C, 1 h). It was due to catalytic synergy of exposed metal active sites, oxygen vacancies (O v ) and acid sites to occur electron transfer and enhance interaction between Pd and ZrO 2 . By tuning the crystal structure of ZrO 2 support, the influence of O v and acid sites of Pd/ZrO 2 over vanillin HDO performance was investigated, Pd/ZS2 with abundant O v and Pd/ZS4 with substantial acid sites promoted hydrogenation and hydrogenolysis , respectively, Pd/ZS3 possessed preferable conversion and selectivity as having the properties of both at once. Additionally, reaction pathway was also proposed in which vanillin was converted to MMP by combining intermediate of 4-hydroxy-methyl-2-methoxyphenol (HMP) with active hydrogen species while removing water. This developed catalysts with different crystalline highlighted an enormous promise for HDO of bio-oils into green fuel under mild conditions.
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高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 24
·16438-16445
·
IF 3.3
Zhiwei Yang,Lijuan Dong,Qian Chen,Zeyi Wang,Jiacheng Cao,Mengwei Dong,Jian Wang,Jian Zhang,Xiao Huang
Although titanium-based MXenes have been widely reported for gas sensing, the effect of crystal stoichiometric variations on the sensing properties has been rarely reported. Herein, stoichiometric polymorphs of titanium carbide MXenes (i.e., Ti3C2Tx and Ti2CTx) loaded with Pd nanodots (NDs) prepared by photochemical reduction were investigated for room-temperature H2 sensing. Interestingly, we found that Pd/Ti2CTx exhibited greatly enhanced sensitivity to H2, along with faster response and recovery rates compared to Pd/Ti3C2Tx. The H2 adsorption induced resistance change in Pd/Ti2CTx was higher than that of Pd/Ti3C2Tx due to the more effective charge transfer at the heterointerface of Pd/Ti2CTx, which was confirmed by shifts of binding energies and theoretical calculation results. We hope this work could be helpful to design more high-performance MXene-based gas sensors.
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高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Fang Wei,Ting Luo,Yan Wang,Lichun Kong,JiuJu Feng,Zhengquan Li,Ji-Qing Lu,Fa Yang
A novel electrocatalyst for CO 2 -to-formate conversion at low overpotentials with abundant bimetallic interfaces aroused from Pd nanoparticles anchoring in the underlying Bi nanosheet (Pd-BiNS) was developed. This unique synthesis procedure undergoes a continuous reconstruction of Pd-BiOINS to Pd-Bi 2 O 2 CO 3 NS to Pd-BiNS, which was confirmed by in situ Raman spectra combined with quasi- in - situ electron microscopy. The optimized Pd 1 -BiNS exhibits a high Faradaic efficiency of 95 % for formate at only − 0.4 V versus reversible hydrogen electrode over 30 h electrolysis, breaking the limitation that metallic Pd-site is easily poisoned by the generated CO at low overpotentials. The in situ infrared spectroscopy indicates that Pd-BiNS has much suppressed *CO binding and enhanced *OCHO adsorption to inhibit the competing hydrogen evolution reaction by repelling surface water molecules, moreover, a systematic CO 2 RR mechanism with HCO 3 − participating as pre-proton donor for formate generation is unveiled. This work provides new insight into the multisite synergistic regulation at the atomic scale.
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高影响因子
FOOD CHEMISTRY
·
2023
·
IF 8.8
Yuhong Li,Yaqi Yang,Yutian Huang,Jiejun Li,Pengcheng Zhao,Junjie Fei,Yixi Xie
Caffeic acid (CA) is widely present in the human daily diet, and a reliable CA detection method is beneficial to food safety. Herein, we constructed a CA electrochemical sensor employing a glassy carbon electrode (GCE) which was modified by the bimetallic Pd-Ru nanoparticles decorated N-doped spongy porous carbon obtained by pyrolysis of the energetic metal–organic framework (MET). The high-energy bond N-N N in MET explodes to form N-doped sponge-like carbon materials (N-SCs) with porous structures, boosting the adsorptive capacity for CA. The addition of Pd-Ru bimetal improves the electrochemical sensitivity. The linear range of the PdRu/N-SCs/GCE sensor is 1 nM-100 nM and 100 nM-15 μM, with a low detection limit (LOD) of 0.19 nM. It has a high sensitivity (55 μA/μM) and repeatability. The PdRu/N-SCs/GCE sensor has been used to detect CA in actual samples of red wine, strawberries, and blueberries, providing a novel approach for CA detection in food analysis.
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高影响因子
Nature Biomedical Engineering
·
2021
·Vol. 6
·期 1
·32-43
·
IF 25.671
Zheng Di-Wei,Deng Wei-Wei,Song Wen-Fang,Wu Cong-Cong,Liu Jie,Hong Sheng,Zhuang Ze-Nan,Cheng Han,Sun Zhi-Jun,Zhang Xian-Zheng
Because a host’s immune system is affected by host–microbiota interactions, means of modulating the microbiota could be leveraged to augment the effectiveness of cancer therapies. Here we report that patients with oral squamous cell carcinoma (OSCC) whose tumours contained higher levels of bacteria of the genus Peptostreptococcus had higher probability of long-term survival. We then show that in mice with murine OSCC tumours injected with oral microbiota from patients with OSCCs, antitumour responses were enhanced by the subcutaneous delivery of an adhesive hydrogel incorporating silver nanoparticles (which inhibited the growth of bacteria competing with Peptostreptococcus ) alongside the intratumoural delivery of the bacterium P. anaerobius (which upregulated the levels of Peptostreptococcus ). We also show that in mice with subcutaneous or orthotopic murine OSCC tumours, combination therapy with the two components (nanoparticle-incorporating hydrogel and exogenous P. anaerobius ) synergized with checkpoint inhibition with programmed death-1. Our findings suggest that biomaterials can be designed to modulate human microbiota to augment antitumour immune responses.
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高影响因子
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