APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Qingqing Wu,Jiaorong Yan,Mingxiang Jiang,Qiguang Dai,Jinyan Wu,Minh Ngoc Ha,Qingping Ke,Xingyi Wang,Wangcheng Zhan
Two-dimensional γ-Al 2 O 3 nanosheet with rich pentacoordinate Al 3+ sites which can nicely stabilize noble metals via strong interactions between metal and support has been focused. However, the synthesis of ultrathin and highly thermal-stable Al 2 O 3 is challenging. Herein, we report an effective approach to synthesize ultrathin Al 2 O 3 nanosheets with regular leaf-like architecture as well as high thermal-stability. A novel intercalation-swelling-exfoliation pathway was proposed to elucidate the formation of ultrathin sheet-like structure and then its morphology/thickness could be further adjusted via a dissolution-growth induced by phosphate. Meanwhile, the presence of phosphate further enhanced thermal stability of Al 2 O 3 nanosheets due to the occupation or depletion of high-reactive sites and surface hydroxy groups. Subsequently, the thermally stable γ-Al 2 O 3 nanosheets with moderate anchoring sites was used as a support of Pd and investigated for catalytic combustion of propane. The Pd/Al 2 O 3 nanosheet exhibited a superior catalytic activity for propane combustion and the complete conversion was below 300 °C, more importantly, the outstanding resistance to high temperature (1000 °C) was observed, which was ascribed to the re-dispersion of Pd particles and the occurrence of strong metal-support interaction (SMSI) at high temperature.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Qiang Zhao,Chiheng Chu,Xin Xiao,Baoliang Chen
The precisely coupling of metal nanoparticles with support domain are crucial to enhance the catalytic activity and stability of supported metal nanoparticle catalysts (MNPs). Here we selectively anchor Pd nanoparticles to the sp 2 domain in graphene-based aerogel constructed with base-washed graphene oxide (BGO) by removing oxidative debris (OD). The effects of OD on the size and chemical composition of Pd nanoparticles in aerogels are initially unveiled. The removal of OD nanoparticles prompt selective coupling of Pd nanoparticles to the exposed sp 2 -hybridized domain on BGO nanosheets, and then prevent it from agglomeration. As a result, the Pd nanoparticle size of self-assembled Pd/BGA is 4.67 times smaller than that of traditional Pd/graphene oxide aerogel (Pd/GA). The optimal catalytic activity of Pd/BGA for the model catalytic reduction of 4-nitrophenol is 15 times higher than that of Pd/GA. Pd/BGA could maintain its superior catalytic activity and achieves 98.72% conversion in the fifth cycle. The superior catalytic performance could be ascribed to the small Pd nanoparticles and high percentage of Pd(0) in Pd/BGA, and the enhanced electronic conductivity of Pd/BGA. These integrated merits of Pd/BGA as heterogeneous catalysts are attributed to selectively anchor Pd nanoparticles on sp 2 -hybridized domain of graphene-based aerogel, and strongly coupled interaction of MNPs with support. The structure-regulated BGO nanosheets could serve as versatile building blocks for fabricating MNPs/graphene aerogels with superior performance for catalytic transformation of water pollutants .
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高影响因子
BIOELECTROCHEMISTRY
·
2020
·
IF 4.722
Qingshan Yang,Ping Wang,Enhui Ma,Haoxuan Yu,Kaiwei Zhou,Chunyuan Tang,Jie Ren,Yueyun Li,Qing Liu,Yunhui Dong
In this work, a sandwich-type electrochemical immunosensor was fabricated to the effective detection of hepatitis B surface antigen (HBsAg). The designed electrochemical immunosensor was based on Au core and Pd shell nanodendrites loaded on amino functionalized molybdenum dioxide nanosheets (Au@Pd NDS/NH 2 –MoO 2 NSs) as the secondary antibody (Ab 2 ) label and silver nanoparticles were loaded by electrodeposited (D-Ag NPs) on the surface of electrode as the platform. Because of the synergistic effect and abundant catalytic activity sites provided by surface dendrite structure, Au@Pd NDs were more effective than single gold and palladium nanoparticles in catalytic reduction of hydrogen peroxide (H 2 O 2 ). MoO 2 had the good catalytic capacity for reduction of H 2 O 2 and favourable electrical conductivity . Hence, the obtained Au@Pd NDS/NH 2 –MoO 2 NSs were more effective than Au@Pd NDs and NH 2 –MoO 2 NSs in catalytic reduction of hydrogen peroxide attribute to a synergistic effect. Also, Ag NPs with admirable electrical conductivity and biocompatibility were used as sensing platforms and primary antibodies (Ab 1 ) carriers, which can accelerate the electron transfer and improve the sensitivity of the immunosensor. Here, the proposed electrochemical immunosensor offered a wide linear interval from 10 fg mL −1 to 100 ng mL −1 and the lower limit of detection of 3.3 fg mL −1 (S/N = 3) for detection of HBsAg under optimal experimental conditions. Furthermore, the accuracy of the actual serum sample analysis was satisfactory, which showed that the electrochemical immunosensor possessed a good application prospect in clinical detection.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
·
IF 7.489
Hao Lei,Qibo Zhang
Construction of strong metal-support interaction (SMSI) is of fundamental interest in the preparation of supported metal nanoparticle catalysts with enhanced catalytic activity. Herein, we report a facile in situ electrochemical redox tuning approach to build strong interactions between metals and supports. As for a typical example, a composite electrocatalyst of Pd-Co hybrid nanoparticles directly developed on Ni substrate is found to follow a distinct surface self-reconstruction process in alkaline media via an in situ electrochemical redox procedure, which results in structural transition from the original nanoparticles (NPs) to nanosheets (NSs) coupled with a phase transformation of the Co component, Co → CoO/Co(OH) 2 . The SMSI is observed in the electrochemically tuned Pd-Co hybrid system and leads to significantly enhanced catalytic activity for methanol oxidation reaction (MOR) due to the modified atomic/electronic structure, increased surface area, and more exposed electroactive sites. Compared with commercial Pd/C catalyst, the electrochemically tuned Pd-Co hybrid catalyst with SMSI exhibits superior catalytic activity (2330 mA∙mg Pd −1 ) and much better stability (remains 503 mA∙mg Pd −1 after 1000 cycles and 172 mA∙mg Pd −1 after 5000 s), and therefore has great potential in practical applications.
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APPLIED CATALYSIS A-GENERAL
·
2020
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IF 5.006
Peng Zhang,Ziyan Wang,Yan Zhang,Jian Wang,Wenqing Li,Lina Li,Peiping Zhang,Cundi Wei,Shiding Miao
In this work a Pd/Fe-Co-Ni layered double hydroxide (LDH) composite was prepared and investigated in the semi-hydrogenation of 2-methyl-3-butyn-2-ol (MBY). Hollow nanocages of ternary Fe-Co-Ni LDH were constructed by stacking the LDH nanosheets edge-to-face which inherited the rhombic dodecahedral structure of ZIF-67 templates. Uniform palladium (Pd) nanocrystals with cubic shapes were imbedded in the LDH nanocages via a solvothermal method. The hydroxyl groups on LDH supports were critical to inhibit the association of excess hydrogen atoms on the catalyst, so less MBY molecules were converted to 2-methyl-2-butanol (MBA) during the hydrogenation catalysis. Under optimized reaction conditions the hydrogenation activity of Pd/Fe-Co-Ni LDH was significantly improved, and the conversion of MBY was higher than 99% with selectivity of 2-methyl-3-buten-2-ol (MBE) exceeding 99%. The catalyst was easily recovered and had little reduction in catalytic performance during the cycling reactions.
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CHEMICAL PHYSICS LETTERS
·
2020
·
IF 2.029
Chunhui Yue,Pan Yang,Jingchuan Wang,Xiaochong Zhao,Yuqi Wang,Lijun Yang
Development of low-cost and high-efficiency catalysts for hydrogen generation represents the significant challenge for realizing hydrogen economy. NiCo and nano-Pd loaded NiCo microfibers with high surface area has been successfully developed by electrospinning and following vacuum thermal treatment. Towards hydrogen generation, the catalyst exhibits efficient TOF as high as 350 and 680 mL min −1 gcat −1 for NiCo and nano-Pd loaded NiCo microfibers, providing superior performance compared with the most promising reported catalysts. The excellent catalytic activity remain above 90% confirming the remarkable durability. The insights uncovered here inspire and guide the rational design of advanced catalysts for the rapidly developing hydrogen energy applications.
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SEMICONDUCTOR SCIENCE AND TECHNOLOGY
·
2020
·Vol. 35
·期 9
·095030
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IF 2.361
Zhiqiang Yao,Xi Wang,Man Yang,He Ma,Yanfeng Sun,Hong Zhang,Tianwei Dong,Weifeng Liu
Doping of noble metals into semiconductors is often used to enhance the response of gas sensors, accompanying the decrease of the particle size. In this work, pure and palladium-doped dispersive nanoscale tin dioxide nanoparticles with abundant surface defects are synthesized efficiently via a facile hydrothermal method. In the experiment, glucose is used as the carbon source to limit the growth of crystals through the carbonization process and create abundant surface defects after high temperature calcination. Compared with pure SnO2, Pd doping only slightly decreases the particle size with the increase of palladium doping amount from 11.9 nm to 9.6 nm. A gas-sensing investigation indicates that the sensor devices based on pure and 1 at%, 3 at%, 5 at% palladium-doped SnO2 show an obvious high response to n-butanol. In particular, the response to n-butanol reaches to the maximum with the palladium doping amount of 3 at%, and the response increases from 33.3 to 92.9 to 100 ppm n-butanol compared with pristine SnO2 nanoparticle at optimal working temperatures. A gas-sensing mechanism related to surface defects, chemical and electrical sensitization is also discussed.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Fangke Zhan,Juanjuan Yin,Anqi Zhang,Jingxin Zhou,Mingli Wang,Tifeng Jiao
A seed-mediated co-reduction (SMCR) method that is simple to operate and produces heterogeneous components by the simultaneous co-reduction strategy to grow crystal was used to prepare a bimetallic nanomaterial, composed of two components of uniform metal elements. In this work, three different cationic surfactants were studied to control the morphology of bimetallic compound materials: cetyltrimethylammonium bromide (CTAB), cetyltrimethylammonium chloride (CTAC), and cetylpyridinium bromide (C16Py). Three mature and stable palladium crystal particles and the same number of Pd–Cu bimetallic nanomaterials (BNMs) products were obtained. The system of Pd and Cu bimetallic components, which has a large lattice mismatch, was grown uniformly by atomic layer-by-layer deposition under the SMCR method. The experimental results of BNMs for two nitro compounds (2-NA and 4-NP) were obtained by UV–vis spectral characterization. The prepared BNMs showed excellent catalytic ability in the reduction reaction and completed the catalytic reaction within 93 s. After eight consecutive catalytic cycles, the conversion of the catalytic reaction reached more than 90%. A set of surface-enhanced Raman scattering (SERS) experiments were also used to test the Raman enhancement properties of these BNMs, demonstrating a good SERS enhancement effect and good uniformity. These research results provide a new research topic for the exploration of morphology-controlled bimetal nanomaterials.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Ming Lei,Zhiying Wang,Yao Tang,Huimin Wang,Lihua Zhu,Heqing Tang
The use of palladium deposited TiO 2 (Pd/TiO 2 ) as catalysts yielded complete debromination of 2,2′,4,4′-tetrabromodiphenyl ether (BDE47) in isopropanol solution containing NaOH at 40 °C within 60 min. The final organic products were diphenyl ether and dibenzofuran. It was disclosed that two competing reduction paths (hydro-debromination and coupling-debromination) occurred over Pd nanoparticles . The hydro-debromination was dependent on the participation of active H atom species generated by catalytic transfer hydrogenation on metallic Pd. The coupling-debromination proceeded via the oxidative addition of Pd(0) to B r 2 C 12 H 8 OB r 2 ′ , leading to an transition state of B r 2 Pd II C 12 H 8 OB r 2 ′ , the reductive dissociation of which resulted in the elimination of Br − ions, producing a new transition state Pd 0 C 12 H 8 OB r 2 ′ − . A further oxidative addition of Pd 0 C 12 H 8 OB r 2 ′ − generated B r 2 ′ Pd II C 12 H 8 O − , and its final reductive elimination provided dibenzofuran, leading to the regeneration of Pd(0). The integration of the catalytic coupling and hydrogenation reaction on Pd nanoparticles greatly accelerated the removal of the halogenated organic pollutants.
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JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Xiqiang Tian,Muhammad Zahid,Jiang Li,Wang Sun,Xiaoyu Niu,Yujun Zhu
The addition of a suitable co-catalyst is an encouraging way to enhance the catalytic performance of Pd based catalyst with low content. Herein, we describe an easy synthesis of Mo 2 N-TiO 2 with well-dispersed Mo 2 N nanoparticles through one pot evaporation-induced self-assembly and nitridation treatment method. Moreover, a green bio-reductive approach with Catalpa Fruit ( CF ) extract was adopted to fabricate Pd/Mo 2 N-TiO 2 catalysts for promoting selective hydrogenation of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) as model reaction. Among these Pd/Mo 2 N-TiO 2 catalysts, 0.8 wt%Pd/Mo 2 N-TiO 2 exhibits significantly high catalytic activity for selective hydrogenation of various nitrophenols and cinnmaldehyde. Importantly, the catalytic activity of the catalyst prepared by the reduction method of the CF extract is higher than that prepared by the reduction method of NaBH 4 . A serials of characterization, including XRD, N 2 adsorption–desorption, TEM, XPS, CO chemisorption and CO-FTIR etc., was carried out to investigate the influence of the prepared method on the surface Pd species and activity. The high performance can be attributed to the specific nanostructure characteristics of the catalyst and the good synergistic effect between Pd and Mo 2 N, improving the dispersion of Pd nanoparticles atoms and the exposure of more active Pd atoms (surface Pd 0 species) on 0.8 wt%Pd/Mo 2 N-TiO 2 due to the CF extract as reductant.
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Nanomaterials
·
2020
·Vol. 10
·期 8
·1612
·
IF 4.324
Zhaoyu Wen,Qiong Fu,Jie Wu,Guangyin Fan
Simple and efficient synthesis of a nano-catalyst with an excellent catalytic property for hydrogen generation from hydrolysis of dimethyl amine-borane (DMAB) is a missing piece. Herein, effective and recycled palladium (Pd) nanoparticles (NPs) supported on soft nitriding porous carbon (NPC) are fabricated and applied for DMAB hydrolysis. It is discovered that the soft nitriding via a low-temperature urea-pretreatment induces abundant nitrogen-containing species on the NPC support, thus promoting the affinity of the Pd precursor and hindering the agglomeration of formed Pd NPs onto the NPC surface during the preparation process. Surface-clean Pd NPs with a diameter of sub-2.0 nm deposited on the NPC support (Pd/NPC) exhibit an outstanding catalytic performance with a turnover frequency (TOF) of 2758 h−1toward DMAB hydrolysis, better than many previous reported Pd-based catalysts. It should be emphasized that the Pd/NPC also possesses a good stability without an obvious decrease in catalytic activity for DMAB hydrolysis in five successive recycling runs. This study provides a facile but efficient way for preparing high-performance Pd catalysts for catalytic hydrogen productions.Keywords:nano-catalyst;dimethyl amine-borane;palladium nanoparticles;hydrolysis;soft nitriding
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高影响因子
FUEL
·
2018
·
IF 4.908
Yanyan Lei,Wenzhi Li,Qingchuan Liu,Qizhao Lin,Xusheng Zheng,Qifu Huang,Shengnan Guan,Xinhua Wang,Chengxin Wang,Fengyu Li
The catalytic efficiency of CeO 2 carriers and the catalytic properties of palladium (Pd) nanocrystals loaded on different morphology CeO 2 carrier were studied for lean methane (CH 4 ) combustion. The catalytic activity of simple CeO 2 carriers was ranked in the order of rod-CeO 2 (r-CeO 2 ) > cube-CeO 2 (c-CeO 2 ) > octahedral-CeO 2 (o-CeO 2 ). After the Pd species was loaded on CeO 2 , 90% of CH 4 was converted at 348 °C catalyzed by Pd/octahedral-CeO 2 (Pd/o-CeO 2 ) with (1 1 1) crystal faces, which had much higher catalytic activity comparing with Pd loaded on c-CeO 2 with (1 0 0) crystal faces and r-CeO 2 with (1 1 0) and (1 0 0) crystal faces. The results of XRD , HRTEM , EDS , H 2 -TPR, XPS and elemental mapping showed that the Pd species in the form of Pd 0 and PdO were highly dispersed on surface of all CeO 2 carriers. Most importantly, quasi In-situ XPS results convinced that Ce 3+ /Ce 4+ ion pairs played an important role in the catalytic combustion of low-concentration methane by adsorbing or releasing oxygen. Compared with r-CeO 2 and c-CeO 2 , the concentration of Ce 3+ on the surface of o-CeO 2 carrier was greatly increased when the Pd species were present, which indirectly reflected that the concentration of oxygen vacancies on the carrier surface also increased. Consequently, the high catalytic activity of Pd/o-CeO 2 is not only related to the high dispersion of Pd 0 and PdO species on the surface of the catalyst, but also closely related to the synergistic interaction between Pd species and (1 1 1) specific faces of o-CeO 2 exposing.
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