ENERGY & FUELS
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2024
·
IF 5.2
Yanbin Zhang,Xifei Yin,Chenghu Zhang,Ying Li,Yinghui Sun,Jie Bai
Dry reforming of methane (DRM) provides an effective method for converting the two main greenhouse gases to hydrogen and carbon monoxide. In this work, Co-CeO2 and CoM-CeO2 (M = Ru, Pd, Pt) catalysts prepared by electrospinning technology were used for DRM. Due to the excellent catalytic performance of Pt itself, the CoPt-CeO2 catalyst had the highest DRM catalytic performance at 850 °C, with a methane (CH4) conversion of 94.12%, and remained stable in 24 h stability testing with almost no carbon deposition. The surface properties of the samples were characterized by Brunauer–Emmett–Teller (BET), temperature programmed reduction with H2 (H2-TPR), temperatureprogrammed desorption of CO2 (CO2-TPD), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). The results indicated that part of the reason for the excellent catalytic performance exhibited by adding noble metals to the catalyst is closely related to the high dispersion of active metals. More importantly, the addition of noble metals significantly increased the medium and strong alkaline sites of the catalysts. The abundant oxygen vacancies in CeO2 itself and the increased alkaline sites of noble metals were conducive to the CO2 adsorption and dissociation and the oxidation of deposited carbon. Moreover, the addition of noble metals promoted the interaction between the active metal and support. The results of this study provide a reference for the design of high-performance Co-based DRM catalysts.
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高影响因子
NANOTECHNOLOGY
·
2015
·Vol. 26
·期 50
·505401
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IF 3.821
Lingyu Tan,Lidong Li,Yi Peng,Lin Guo
Herein, a new type of uniform and well-structured Au@Pt bimetallic nanoparticles (BNPs) with highly active concave Au nanocuboids (NCs) as seeds was successfully synthesized by using the classic seed-mediated method. Electrochemical measurements were conducted to demonstrate their greatly enhanced catalytic performance in the ethanol oxidation reaction (EOR). It was found that the electrochemical performance for Au@Pt BNPs with the concave Au NCs as seeds, which were enclosed by {611}high-index facets, could be seven times higher than that of the Au@Pt bimetallic nanoparticles with regular spherical Au NPs as seeds. Furthermore, our findings show that the morphology and electrocatalytic activity of the Au@Pt BNPs can be tuned simply by changing the compositional ratios of the growth solution. The lower the amount of H2PtCl6 used in the growth solution, the thinner the Pt shell grew, and the more high-index facets of concave Au NCs seeds were exposed in Au@Pt BNPs, leading to higher electrochemical activity. These as-prepared concave Au@Pt BNPs will open up new strategies for improving catalytic efficiency and reducing the use of the expensive and scarce resource of platinum in the ethanol oxidation reaction, and are potentially applicable as electrochemical catalysts for direct ethanol fuel cells.
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Applied Catalysis O: Open
·
2024
·
IF 0
Ya-Song Lin,Hui-Zi Han,Xiao-Qi He,Xian-Tai Zhou
A highly efficient and selective protocol for the oxidation of alkyl aromatics with tert -butyl hydroperoxide (TBHP) oxidant over platinum meso -tetraphenylporphyrin (Pt( II )TPP) was developed. Various alkyl aromatics were selectively converted to ketones smoothly with yields higher than 90% under the optimized conditions. Kinetic studies revealed that the oxidation was first-order with respect to the substrate, and the activation energy ( E a ) was 50.8 kJ mol −1 . Moreover, a mechanism involving high-valence platinum species and free radicals was proposed.
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JOURNAL OF POWER SOURCES
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2024
·
IF 8.1
Jirong Yang,Chaoyang Shi,Feng Liu,Enze Zhu,Danyang Wei,Yanrong Ren,Rui Chen,Mingli Xu
The construction of an integrated electrode with self-organized growth is of great significance in reducing the Pt loading and improving the performance of the membrane electrode assembly (MEA) in proton exchange membrane fuel cells (PEMFCs). Herein, the square-wave pulse electrodeposition method is used to grow Pt {510}CNC and Pt {720}CNC nanocrystals on carbon fiber paper (CFP)-based reduced graphene oxide (rGO/CFP) and nitrogen-doped reduced graphene oxide (N-rGO/CFP) supports, respectively. Experimental and density functional theory (DFT) calculations show that the introduction of N makes it easier for hydrogen to adsorb on Pt, and the arrangement order of more Pt atoms is disrupted by hydrogen, resulting in the formation of Pt concave nanocubes (Pt CNCs) with small interface angles (α), consisting of {720} facets with more atomic steps. Moreover, the catalytic activities of the prepared two catalysts for methanol oxidation are 3.17 and 2.35 times higher than that of commercial Pt/C, and the maximum power densities of direct methanol fuel cell (DMFC) are also better than that of commercial Pt/C. This work can provide important guidance for the future research of high-index facets noble metal nanocrystals for growth on the surface of defective carbon carriers as integrated electrodes in MEA.
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ACS Sensors
·
2020
·
IF 7.333
Wei Chen,Lijun Yang,Chao Yan,Bangben Yao,Jianfeng Lu,Jianguo Xu,Guodong Liu
Overuse and abuse of morphine (MOP), one of the main components of pericarpium papaveris, have attracted increasing attention in the medical field owing to its pharmacological and toxicological activity. Herein, we proposed a new electrochemical nano-biosensor for MOP detection based on surface-confined building of Au@Pt-centered and multi-G-quadruplex/hemin wire-surrounded electroactive super-nanostructures. The center Au@Pt was flower-shaped and irregularly protruded, allowing substantial loading of multiple G-quadruplex wire/hemin complexes on its surface to accomplish the assembly of electroactive super-nanostructures. Interestingly, as the super-nanostructures were closely confined on the electrode surface, a significantly amplified electrochemical signal was thus obtained in the absence of MOP. In contrast, the introduction of target MOP can induce an intense competitive effect and strongly destroy the assembly process, resulting in the reduction of the electrochemical response that is correlated with the logarithmic concentration of MOP. Under optimal conditions, the electrochemical nano-biosensor is capable of highly sensitive detection of MOP in a dynamic concentration range from 1 ppt to 500 ppb. The limit of detection is achieved as low as 0.69 ppt, and the practical application was confirmed by examining MOP from chafing dish condiments. We expect the electrochemical platform utilizing this unique nanoarchitecture to provide rational guidelines to design high-performance analytical tools.
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Journal of Physical Chemistry C
·
2012
·
IF 4.805
Jian Zhao,Liqing Zhang,Tao Chen,Hui Yu,Lin Zhang,Hao Xue,Haiqing Hu
A combination of graphene with metal particles is particularly attractive due to the enhanced performance of the hybrid materials. However, direct loading of uniform metal nanoparticles such as Pt on graphene remains a challenge due to the hydrophobic nature of graphene. We herein demonstrate that Pt nanoparticles with uniform size and high dispersion were deposited on graphene surfaces via a facile and efficient supercritical fluid method. The graphene sheets used in this work were produced by rapid thermal expansion of graphite oxide. With the help of supercritical carbon dioxide (SC CO2), Pt nanoparticles with a mean size of 3.28 nm are evenly distributed on graphene upon the reduction of an organic platinum precursor. The electrocatalytic investigations reveal that the current density of methanol electrooxidation with the resultant Pt/graphene catalyst was ∼3.5 times as large as that observed with conventional Pt/carbon black (Vulcan XC-72) catalyst. The results demonstrate that graphene serves as an excellent electrocatalytic carrier, and the supercritical fluid strategy is powerful and promising for the synthesis of highly active electrocatalysts for direct methanol fuel cells.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Ying Duan,Pan Guo,Dong Sui,Dongsheng Deng,Tianliang Lu,Yanliang Yang
The development of a cost-effective catalyst for hydrogen evolution from ammonia borane is of importance for the application of AB as a hydrogen storage material. In this manuscript, a series of noble metal catalysts M@CuOx/C (M = Ru, Rh, Pd, and Pt) are prepared by the galvanic reduction method. The catalysts are characterized by XRD , TEM , EDS mappings and lines scanning, XPS , HAADF-STEM, and ICP-OES. The noble metal is highly dispersed on the surface of Cu nanoparticles . The morphology of Cu nanoparticles changed according to different metals after the introduction of noble metal and there has an interaction between the noble metal and Cu. The M@CuOx/C is used for the hydrolysis of AB. For the same metal catalyst, the activity of M@CuOx/C is increased by about 3–7 times than the corresponding M/C at 298 K. The Rh shows the highest TOF and lowest activation energy among the four noble metals.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xing Qian,Chong Xu,Yiqing Jiang,Jie Zhang,Guoxiang Guan,Yixuan Huang
Multi-shelled micro-/nanomaterials with complex hollow structures have been regarded as a promising kind of advanced catalysts for energy conversion owing to their large specific surface, increased active sites, and shortened paths of charge transfer. Herein, a series of double-shelled transition metal chalcogenides (Ni-Co-MoS x , Co-MoS x , and Ni-MoS x ) with ball-in-ball hollow structures have been synthesized by converting corresponding metal-glycerol spherical precursor with the assistance of (NH 4 ) 2 MoS 4 under a facile solvothermal condition. In this process, (NH 4 ) 2 MoS 4 acted as a multifunctional vulcanizator, which could conveniently afford Mo and S elements at the same time, and the mass ratio of the precursor to (NH 4 ) 2 MoS 4 played an indispensable role in preparing the uniform hollow sphere with satisfactory morphology and catalytic performance. Noteworthily, compared with ternary Co-MoS x and Ni-MoS x , the quaternary Ni-Co-MoS x ball-in-ball nanospheres demonstrated much enhanced catalytic properties in accelerating the reduction of triiodide in dye-sensitized solar cells (DSSCs) and the electrochemical hydrogen evolution reactions (HERs) due to the advantages of multi-elements, moderated surface texture, and larger surface area. Specifically, a prominent power conversion efficiency of 9.63% was achieved by the DSSC assembled with Ni-Co-MoS x counter electrode (CE), which was much superior to that of Pt CE (8.28%). Besides, Ni-Co-MoS x showed a low η 10 of 93.4 mV and a small Tafel slope of 55.0 mV dec −1 when employed as electrocatalysts for HER in 0.5 M H 2 SO 4 .
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NANOTECHNOLOGY
·
2020
·Vol. 31
·期 18
·185701
·
IF 3.551
Xiaofeng Cui,Yu Zhou,Jian Wu,Shan Ling,Lijun Zhao,Jianli Zhang,Junwei Wang,Wei Qin,Yuanguang Zhang
A solid-state Z-scheme system, with the synergistic integration of the advantages of various narrow-band semiconductors, is considered to be a potential strategy to develop efficient photocatalysts for operation under visible light illumination. However, the charge separation efficiency of these systems has always been reduced by disordered electron transfer between coupling semiconductors. In this work, we constructed a direct Z-scheme system WO3-MoS2-Pt through the loading of WO3 quantum dots onto MoS2 nanosheets and the selective depositing of a Pt co-catalyst onto MoS2. X-ray diffraction, transmission electron microscopy, atomic electron microscopy and x-ray photoelectron spectroscopy, etc were used to confirm the successful preparation of the targeted photocatalyst. This photocatalytic system showed high visible-light-driven H2 evolution activity (802.2 μmol · h−1 · g−1) and good photostability. Control experiment and mechanism analysis suggested that the remarkable performance can be attributed to the heterojunction formed WO3 and MoS2 and the vectorial electron transfer (WO3 → MoS2 → Pt) achieved by selectively loading the Pt co-catalyst.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Min Li,Feng Liu,Yongming Zhang
It is challenging to synthesize oxygen reduction reaction (ORR) electrocatalysts that are highly efficient, affordable, and stable for use in proton exchange membrane fuel cells. To address this challenge, we developed a low platinum-loading (only 6.68% wt) ORR catalyst (PtCu1-NC), comprising CuPt nanoparticles (average size: 1.51 nm) supported on the N-doped carbon substrates. PtCu1-NC possesses a high specific surface area of 662 m2 g–1 and a hierarchical porous structure, facilitating efficient mass transfer. The synergistic effect from introduced copper and the electron effect from nitrogen modify the electronic structure of platinum, effectively accelerating the ORR reaction and enhancing stability. Density functional theory calculations demonstrate the catalytic mechanism and further verify the synergistic effect. Electrochemical assessments indicate that PtCu1-NC exhibits specific activity and mass activity 5.3 and 5.6 times higher, respectively, than commercial Pt/C. The half-wave potential is 27 mV more positive than that of commercial Pt/C. The electrochemical active surface area value is 104.3 m2 g–1, surpassing that of Pt/C. Approximately 78% of current is retained after 10,000 s chronoamperometry measurement. These results highlight the effectiveness of alloying in improving the catalyst performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Shujun Qiu,Yongli Shen,Guijuan Wei,Shuang Yao,Wei Xi,Miao Shu,Rui Si,Min Zhang,Junfa Zhu,Changhua An
Maximizing the usage of cocatalyst to provide fruitful proton reduction sites and suppress charge carrier recombination is an effective stratagy to dramatically improve the photocatalytic performance. Herein, anchoring single atoms (SAs) of Pt onto the ultrathin porous CdS@carbon dots (CDs) nanosheets has been achieved through in-situ reduction of Pt precursor. X-ray absorption fine structure spectra identify that the single Pt atoms are bonded as Pt-S with a coordination number 4, due to the scattering between platinum center and the sulfur atoms. The Pt single atoms exhibit strong capacity to trap photo-generated electrons, rendering CdS@CDs/Pt-SAs as a class of efficient solar-driven photocatalyst. It shows an outstanding activity towards H 2 generation at rate of 45.5 mmol h −1 g −1 , which is 133 times of that for bare CdS@CDs. The novel method can be extended to the preparation of various functional nanocatalysts owing to its versatility and facileness.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Wei Bi,Yanjie Hu,Wenge Li,Hao Jiang,Chunzhong Li
In this work, a nanoreactor combining layers of facile traditional two-dimensional (2D) material, hexagonal boron nitride (h-BN, which often called the white graphene) with Pt/Al2O3 catalyst was designed to exhibit higher stability, activity, and selectivity in automobile exhaust treatment. Characterization revealed that h-BN does coat on the surface of platinum and forms a distinct Pt@h-BN/Al2O3 core–shell nanostructure. This as-prepared catalyst possesses good thermal stability and selectivity, because of the excellent high-temperature tolerance and the multidefected structure of the h-BN shell; that is, small molecules such as CO and O2 can easily intercalate into the nanoreactor, while large molecules such as propylene are blocked out. Meanwhile, the intercalated reactants can achieve the conversion of CO to CO2 faster (ΔT100 = 20 °C) with the confinement effect. The study indicates that constructing a nanoscale confined environment with two-dimensional (2D) coating can enhance the performance of the catalyst in multiple aspects and simultaneously provide a good example for designing nanostructured catalysts with multifaceted improvement.
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