JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Jiansong Wang,Yangyang Yu,Wenkai Xu,Hui Yu,Weiwei Zhang,Hongliang Huang,Gui-Rong Zhang,Donghai Mei
Ammonia borane (AB) represents a promising hydrogen storage material, while high-performing catalysts allowing efficient release of hydrogen from the hydrolysis of AB are desired. Here, Pd nanoclusters (NCs) are successfully immobilized within pores of a bipyridyl covalent triazine framework (CTF-BPDA-TPDH) via a metal-nitrogen coordination reduction strategy. The porous structure and tailored N sites of CTF facilitate the anchoring of Pd ions and the in situ formation of monodisperse Pd NCs confined in the pores of CTF. The resulting Pd-NCs@CTF composites exhibit high activity toward the hydrolysis of AB with turnover frequencies (TOFs) of 273 and 434 mol H2 ·mol −1 Pd ·min −1 in neutral and alkaline solutions, respectively. The Pd-NCs@CTF catalyst is also demonstrated for the tandem dehydrogenation of AB and hydrogenation of nitroarenes featuring short reaction time and high yields. These findings emphasize the promise of the porous CTFs encapsulated metal NCs for active catalysts.
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Catalysts
·
2022
·Vol. 12
·期 5
·528
·
IF 4.501
Chuxuan Pan,Yuanyuan Zheng,Jing Yang,Dongyang Lou,Jian Li,Yujing Sun,Wei Liu
Hydrogen peroxide (H2O2) plays an indispensable role in the biological, medical, and chemical fields. The development of an effective H2O2detecting method is of great importance. In the present work, a series of PtxPdybimetallic aerogels and Pt, Pd monometallic aerogels were controllably synthesized by one-step gelation method. Their morphologies and compositions were characterized by transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy, and so forth. These aerogels were used as nonenzyme electrocatalysts for the detection of H2O2. The cyclic voltammetric and amperometric results demonstrated that the performance of the metal aerogels showed volcano-type behavior, with the Pt50Pd50aerogel sitting on top. The Pt50Pd50aerogel-based electrochemical sensor exhibited excellent comprehensive performance, with a low overpotential of −0.023 V vs. Ag/AgCl, a broad linear range from 5.1 to 3190 μM (R2= 0.9980), and a high sensitivity of 0.19 mA mM−1cm−2, in combination with good anti-interference ability and stability. A comprehensive study indicated that the superior sensing performance of the Pt50Pd50aerogel is closely related to its optimized d-band center and larger cumulative pore volume. This work first applied Pt–Pd bimetallic aerogels into the detection of H2O2and shows the promising application of noble metal aerogels in the electrochemical sensing area.Keywords:electrochemical sensors;hydrogen peroxide;electrocatalysis;alloying effect
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Zhefei Zhao,Li Yu,Lingxia Zheng,Tianyang Guo,Zhuoqing Lv,Shuang Song,Huajun Zheng
The development of catalysts with high atom utilization and activity is the biggest challenge for electrocatalytic hydrodechlorination (EHDC) technology . Herein, a design strategy of TiO 2 @PDA inorganic-organic core-shell skeleton for loading lower dosage of noble palladium (Pd) with robust activity is reported. The self-supported TiO 2 @PDA nanorod arrays provides exposed surface area for anchoring Pd and PDA as interlayer controls the Pd nucleation to form nanodots with high dispersion, realizing high atom utilization. Moreover, the strong interaction between PDA and Pd realizes the coexistence of electron-rich and deficient Pd species with suitable proportion, which facilitate the H* formation and the C-Cl bond activation, respectively, resulting in the promoted activity. The optimal TiO 2 @PDA/Pd electrode exhibits a low dosage of Pd (0.093 mg cm −2 ) and excellent activity for 4-chlorophenol reduction with a mass activity (MA) of 23.96 min −1 g −1 , which is 3.31 times as high as that of TiO 2 /Pd. The design scheme with inorganic-organic core-shell skeleton as support is benefit for developing highly efficient and lower price elctrocatalysts for EHDC.
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Applied Materials Today
·
2022
·
IF 8.663
Ruirui Zhang,Liping Zhong,Xiuli Liu,Xiyu Liu,Qiaoying Chen,Pan Wu,Jian He,Yongmei Li,Yongxiang Zhao,Ziqun Liu,Yan Zu,Yong Huang,Bing Wang
Immunotherapy has made encouraging progress in the field of cancer treatment. Among them, the programmed cell death-ligand 1 (PD-L1) antibody-mediated immunotherapy has stimulated the development of various carrier delivery systems. Inspired by related researchs, in this study, we prepare core-shell structured poly(lactide-co-glycolide) (PLGA) microcapsules as a drug delivery system through microfluidics technology, loaded with PD-L1 aptamers and chemotherapy drug docetaxel. The PD-L1 aptamer loaded in the nuclear layer binds to the PD-L1 molecule produced by tumor cells, blocking the immune checkpoint protein-1/programmed cell death-ligand 1 (PD-1/PD-L1) pathway. As a result, phagocytosis of tumor cells is promoted by using lipopolysaccharide (LPS) induced tumor associated macrophages. Furthermore, docetaxel in the shell is further released, inhibiting tumor cell growth as the PLGA microcapsules degrade. More importantly, the combination of PD-L1 aptamers and the chemotherapy drug docetaxel improved the immune response of the tumor. It showed significant anti-tumor activity and reduced systemic side effects in the melanoma model. At present, more and more nucleic acid aptamers as affinity reagents that can replace antibodies have been used to improve tumor treatment. Therefore, this therapeutic strategy provides more possibilities for tumor treatment by combining aptamer molecules with chemotherapy drugs when exploring more effective combination drugs.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2022
·
IF 3.898
Lu Lv,Min Zhao,Yanan Liu,Yufei He,Dianqing Li
Alumina (Al 2 O 3 ) is widely used in the chemical industry as the catalyst and support due to its high specific surface area, abundant pore size distribution and chemical stability. However, the occurrence of hydration in water environment, result in outstanding decrease in specific surface area and collapse of pore structure. In this work, dodecyl phosphoric acid (PA) is used to modify the surface of Al 2 O 3 to obtain a series of hydrophobic material (Al 2 O 3 -PA). Based on XPS and NMR analysis, PA is chemically bonded on Al 2 O 3 to form P O Al bond. Furthermore, BET and WCA results display that Al 2 O 3 -1PA exhibits excellent the hydrophobicity and hydrothermal stability while maintains the pore structure. Take it as the substrate to support the Pd nanoparticles , the as-prepared Pd/Al 2 O 3 -PA shows the superior catalytic performance in the hydrogenation of phenol and anthraquinone relative to Pd/Al 2 O 3 , indicating the accessibility of Pd sites after PA modification. Especially, the significantly enhanced stability is also obtained in four cycles for aqueous phenol hydrogenation. This can be ascribed that the PA modification inhibits the aggregation of Pd nanoparticles and the products adhesion in the reaction process. The extension of PA coatings to monolithic catalysts could expand their current capabilities in industrial applications and warrants ongoing investigation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Yanju Chen,Chao Feng,Wenhong Wang,Zhi Liu,Junxi Li,Chenguang Liu,Yuan Pan,Yunqi Liu
Regulating the electronic structure of Pd catalyst for promoting electrocatalytic hydrodechlorination is promising but still challenging. Herein, we propose an electronic structure engineering for accelerating the hydrodechlorination process by desigining bimetallic Pd-Au alloy nanoparticles (ANs) with electron-rich Pd as high-efficiency electrocatalysts. The Pd 7 Au 3 ANs exhibits the highest electrocatalytic hydrodechlorination activity, the 4-chlorophenol hydrodechlorination efficiency reaches 98.35 % within 4 h, and the mass activity is 0.47 h −1 mg Pd −1 , which is 7.83 times as high as that of pure Pd nanoparticles. The experimental characterization and theoretical calculation reveal that Pd atoms “obtain” electrons and gold atoms “lose” electrons in Pd-Au ANs, resulting in the formation of electron-rich Pd, which promotes the desorption of the dechlorination product phenol and accelerates the renewal of active sites. This work provides an electronic structure engineering strategy of Pd-based electrocatalysts for electrocatalytic hydrodechlorination, which opens a new opportunity for rational design and construction of high-performance hydrodechlorination catalysts.
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Xiaoning Meng,Mingshu Bi,Qiuping Xiao,Wei Gao
With the emergence of hydrogen economy worldwide and the increase of safety problems caused by the highly flammable and explosive characteristics of hydrogen (H 2 ), it is urgent to develop the portable sensors that can sensitively and quickly detect H 2 leaks. In this work, the H 2 sensing characteristics of Pd/SnS 2 /SnO 2 nanocomposites synthesized via hydrothermal route as well as impregnation route were systematically investigated for the first time. The influence of different SnS 2 and Pd loading on the H 2 sensing performances of SnO 2 nanoparticles was revealed by varying the addition levels of thiourea and palladium chloride. The H 2 sensing experimental results demonstrated that SnS 2 and Pd modification can greatly enhance the sensing capabilities of SnO 2 , where 1.0 at% Pd/SnS 2 /SnO 2 sensor exhibited high response (95) and rapid response/recovery time (1/9 s) to 500 ppm H 2 at 300 ℃, thus outperforming the current reported sensing performances of SnO 2 -based H 2 sensors. The superior sensing characteristics of Pd/SnS 2 /SnO 2 were attributed to the simultaneous synergistic effect of the three components. This study will supply a rational strategy for designing high sensitive and rapid response H 2 sensors.
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Materials
·
2022
·Vol. 15
·期 4
·1367
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IF 3.748
Fubing Gui,Yong Huang,Menghan Wu,Xilai Lu,Yongming Hu,Wanping Chen
A high long-term stability is crucial for room-temperature gas-sensitive metal oxide semiconductors (MOSs) to find practical applications. A series of Pd-SnO2mixtures with 2, 5, and 10 wt% Pd separately were prepared from SnO2and Pd powders. Through pressing and sintering, Pd-SnO2composite nanoceramics have been successfully prepared from the mixtures, which show responses of 50, 100, and 60 to 0.04% CO-20% O2-N2at room temperature for samples of 2, 5, and 10 wt% Pd, respectively. The room-temperature CO-sensing characteristics were degraded obviously after dozens of days’ aging for all samples. For samples of 5 wt% Pd, the response to CO was decreased by a factor of 4 after 20 days of aging. Fortunately, some rather mild heat treatments will quite effectively reactivate those aged samples. Heat treatment at 150 °C for 15 min in air tripled the response to CO for a 20 days-aged sample of 5 wt% Pd. It is proposed that the deposition of impurity gases in air on Pd in Pd-SnO2composite nanoceramics has resulted in the observed aging, while their desorption from Pd through mild heat treatments leads to the reactivation. More studies on aging and reactivation of room-temperature gas sensitive MOSs should be conducted to achieve high long-term stability for room-temperature MOS gas sensors.Keywords:CO;sensors;SnO2;aging;heat treatment;recover
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Asian Journal of Organic Chemistry
·
2023
·Vol. 12
·期 7
·e202300216
·
IF 2.7
Yi-Ying Zhuang,Xiao-Chao Chen,Kai-Chun Zhao,Guo-Sheng Zhang,Yu-Fen Xie,Yong Lu,Ye Liu
Graphical Pd-catalyzed anti -Markovnikov hydrocarboxylation of vinylarenes with formic acid free of auxiliary additive has been reported. This work was financially supported by the National Natural Science Foundation of China (Nos. 22172052 and 21972045), and the Research Funds of Happiness Flower ECNU (2022ST2203).
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 19
·10222-10227
·
IF 11.9
Ziqiang Wang,Guanghui Yang,Pengjun Tian,Kai Deng,Hongjie Yu,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Water electrolysis for hydrogen production consumes abundant electronic energy owing to the sluggish oxygen evolution reaction (OER), so the integration of the hydrogen evolution reaction (HER) with thermodynamically more favorable oxidation reactions is a promising strategy for energy-efficient hydrogen production. Herein, we propose the epitaxial confinement of rhodium nanoparticles (NPs) to palladium metallene (Rh/Pd metallene) for hydrogen production assisted by the hydrazine oxidation reaction (HzOR). The two-dimensional structure of Rh/Pd metallene provides sufficient active sites as well as a rapid charge transfer rate. The interface of Pd metallene with Rh NPs ensembles to modulate the electronic state, thus optimizing the adsorption energy of reaction intermediates. The Rh/Pd metallene exhibits splendid HER and HzOR activities, with overpotentials of 59 and 7 mV at 10 mA cm−2, respectively. In the two-electrode construction of a hydrazine oxidation-assisted water splitting system, the Rh/Pd metallene only needs a low overpotential of 0.19 V to produce hydrogen at a current density of 100 mA cm−2. This research offers a viable approach for designing nanosheet/nanoparticle heterojunction as an attractive modular platform for energy-saving hydrogen production.
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JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Jing Zhang,Weiqi Liao,Hao Zheng,Yunshang Zhang,Lebing Xia,Bo-Tao Teng,Ji-Qing Lu,Weixin Huang,Zhenhua Zhang
Pd supported on different anatase TiO 2 nanocrystals predominantly exposing either {1 0 0}, {1 0 1}, or {0 0 1} facets were tested for CO 2 hydrogenation into formate. Remarkable morphology-dependent catalysis was observed. Compared to 2%Pd/TiO 2 {1 0 1} and 2%Pd/TiO 2 {0 0 1} catalysts, 2%Pd/TiO 2 {1 0 0} is highly active and stable, affording an unprecedented turnover frequency of ca. 1369 h −1 and keeping stable after 6 cycles at 313 K. This can be associated with, on the one hand, higher density of moderate basic site and relatively more Pd(0) species over 2%Pd/TiO 2 {1 0 0} contribute to the activations of CO 2 and H 2 , respectively, favorable for the activity; On the other hand, higher oxygen vacancy concentrations in the TiO 2 {1 0 0} promote the Pd-TiO 2 interactions and result in the formation and stability of flat Pd particles over 2%Pd/TiO 2 {1 0 0}, beneficial to the stability. These results highlight the importance of oxide morphology in formate formation and open up possibilities of oxide morphology engineering for developing efficient Pd-based catalysts for CO 2 hydrogenation.
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Acta Biomaterialia
·
2021
·
IF 8.947
Zefeng Wang,Yanling Peng,Yan Zhou,Shengnan Zhang,Jianxi Tan,Huan Li,Dinggeng He,Le Deng
Photothermal therapy (PTT) is a promising strategy for antimicrobial therapy. However, the application of PTT to treat bacterial infections remains a challenge as the high temperature required for bacterial elimination can partly damage healthy tissues. Selecting the appropriate treatment temperature is therefore a key factor for PTT. In this work, we designed a near-infrared/pH dual stimuli-responsive activated procedural antibacterial system based on zeolitic imidazolate framework-8 (ZIF-8), which was bottom-up synthesized and utilized to encapsulate both Pd-Cu nanoalloy (PC) and the antibiotic amoxicillin (AMO). This procedural antibacterial therapy comprises chemotherapy (CT) and PTT. The former disrupts the bacterial cell wall by releasing AMO in an acidic environment, which depends on the sensitive response of ZIF-8 to pH value change. With the progression in time, the AMO release rate decreased gradually. The latter can then significantly stimulate drug release and further complete the antibacterial effect. This impactful attack consisted of two waves that constitute the procedural therapy for bacterial infection. Accordingly, the treatment temperature required for antibacterial therapy can be significantly lowered under this mode of treatment. This antibacterial system has a significant therapeutic effect on planktonic bacteria (G + /G − ) and their biofilms and also has good biocompatibility; thus, it provides a promising strategy to develop an effective and safe treatment against bacterial infections. Statement of Significance We have developed a near infrared/pH dual stimuli-responsive activated procedural antibacterial system that combines enhanced antibiotic delivery with photothermal therapy and has highly efficient antimicrobial activity . The antibacterial effect of this therapy was based on two mechanisms of action: chemotherapy, in which the bacterial cell wall was first destroyed, followed by photothermal therapy. After exposure to irradiation with an 808 nm laser, the inhibition rates were 99.8% and 99.1% for Staphylococcus aureus and Pseudomonas aeruginosa , respectively, and the clearance rates for their established biofilms were 75.3% and 74.8%, respectively. Thus, this procedural antibacterial therapy has shown great potentiality for use in the photothermal therapy of bacterial infectious diseases, including biofilm elimination.
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