DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 11
·3325-3332
·
IF 4
Rongqian Cui,Jiaqi Zhou,Dan Wang,Yafei Zhao,Xu Xiang,Huishan Shang,Bing Zhang
The development of highly active, low cost and durable catalysts for selective hydrogenation of aldehydes is imperative and challenging. In this contribution, we rationally constructed ultrafine Pt nanoparticles (Pt NPs) supported on the internal and external surfaces of halloysite nanotubes (HNTs) by a facile double solvent strategy. The influence of Pt loading, HNTs surface properties, reaction temperature, reaction time, H2 pressure and solvents on the performance of cinnamaldehyde (CMA) hydrogenation was analyzed. The optimal catalysts with the Pt loading of 3.8 wt% and the average Pt particle size of 2.98 nm exhibited outstanding catalytic activity for the hydrogenation of CMA to cinnamyl alcohol (CMO) with 94.1% conversion of CMA and 95.1% selectivity to CMO. More impressively, the catalyst showed excellent stability during six cycles of use. The ultra-small size and high dispersion of Pt NPs, the negative charge on the outer surface of HNTs, the –OH on the inner surface of HNTs, and the polarity of anhydrous ethanol solvent account for the outstanding catalytic performance. This work offers a promising way to develop high-efficiency catalysts with high CMO selectivity and stability by combining clay mineral halloysite and ultrafine nanoparticles.
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高影响因子
SOLAR ENERGY
·
2022
·
IF 7.188
Kai Sheng,Mahmoud A. Khalifa,Zitao Wang,Jianming Zheng,Chunye Xu
Developing a low-cost and efficient Photovoltachromic Device (PVCD) can address the requirements of energy-harvesting smart windows . In this work, low-cost poly(3,4-(2,2-dimethylpropylenedioxy)thiophene) (PProDOT-Me 2 ) is presented for replacing expensive Pt and achieving a WO 3 -based PVCD with rapid bleaching speed. The device consists of the proposed WO 3 /PProDOT-Me 2 electrode, an electrolyte containing I − /I 3 − redox couple , and dye-sensitized TiO 2 photoanode. The PVCD changes state between colored and bleached by simply altering the open and short circuit of the device. The PVCD achieves high optical contrast of 45.1% at 680 nm with a fast bleaching time of 15.5 s, coloring time of 3.6 s, and cycling stability over 200 cycles. These unique characteristics result from the PProDOT-Me 2 could help accelerate the electrochromic process of WO 3 and fast transferring charges to the electrolyte that enhances photovoltaic performance . The accelerating mechanism is analyzed and the related experimental evaluations are executed. This study reveals promising prospects of the proposed WO 3 -PProDOT-Me 2 electrode for low-cost PVCD.
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AICHE JOURNAL
·
2022
·Vol. 68
·期 7
·e17677
·
IF 4.167
Shen Hu,Jiaxuan Chen,Qunfeng Zhang,Junru Liu,Jinlin Meng,Guanghua Ye,Xinggui Zhou,Weikang Yuan
Surface barriers persist in the molecular transport across external crystal surface of zeolites, which brings strong influences on zeolite catalysis. This study probes the role of crystal-size–dependent surface barriers in zeolite catalysis, with n -pentane isomerization catalyzed by Pt/ZSM-5 as a model reaction system. Chemical liquid deposition of SiO 2 is performed to reduce surface barriers on ZSM-5 crystals with different sizes. After SiO 2 deposition, surface barriers on both small (266 nm) and large (1304 nm) crystals are significantly reduced, while the improvement in catalytic activity for the large crystals (76.1%–129.1%) is much higher than that for the small ones (−17.4% to 16.7%). For the large ZSM-5 crystals, diffusion limitation is stronger, and thus the effect of surface barriers on catalytic activity is more important. This study reveals the unique role of crystal-size–dependent surface barriers in zeolite catalysis, and understanding this is important for the optimal design of zeolite catalysts.
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SENSORS AND ACTUATORS A-PHYSICAL
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2022
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IF 4.291
Jing Li,Guoyun Zhou,Yan Hong,Wei He,Shouxu Wang,Yuanming Chen,Chong Wang,Yao Tang,Yukai Sun,Yongkang Zhu
Wearable electronic devices with biocompatibility and stability to monitor the practical human physiological states are urgently expected for some intensive disease recovery or healthy fitness improvement. In this work, a highly sensitive piezoelectric sensor with the aid of polythiophene (PT) promoting polyvinylidene Fluoride (PVDF) from α-phase to β-phase was designed. Electric-sensitivity of 4.961 V/N is obtained at the low-pressure and 0.09 N periodic pressure positively produces considerable output open circuit voltage. It is proved that PT facilitates PVDF to accumulate charge carriers at their interfaces, resulting in interface polarization and thus extremely piezoelectric sensitivity. Reliability test suggested the sensor stays stable performance after a long-term (~2.6% decline after 5000 cycles) repetitive deformation. Through the practices of our assembled wearable sensor demonstrating its powerful ability in recording human joint movement and breathing, which also shows that it is very promising in online movement monitoring of personal health.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Huiyi Yang,Qiyi He,Mingxia Lin,Li Ji,Leheng Zhang,Huanxin Xiao,Shijia Li,Qinglan Li,Xiping Cui,Suqing Zhao
Multimodal lateral flow immunoassay (LFIA) has displayed its potential to improve practicability and elasticity of point-of-care testing. Herein, multifunctional core-shell-shell Au@Pt@Ag NPs loaded with dual-layer Raman reporter molecules of 5,5′-dithiobis-(2-nitrobenzoic acid) (DTNB) with a characteristic combination of color-photothermal-Raman performance were constructed for colorimetric LFIA (CM-LFIA), photothermal LFIA (PT-LFIA) and surface-enhanced Raman scattering-based LFIA (SERS-LFIA), respectively. The highly specific nanoprobes , being obtained through the combination of the resulted dual-layer DTNB modified Au@Pt@Ag NPs with the antibody, were triumphantly utilized in exploring multimodal LFIA with one visual qualitative and two optional quantitative modes with excellent sensing sensitivity. Under optimal conditions, the limit of detection (LOD) for the model hazardous analyte dehydroepiandrosterone (DHEA) were 1.0 ng mL −1 for CM-LFIA, 0.42 ng mL −1 for PT-LFIA, and 0.013 ng mL −1 for SERS-LFIA, three of which were over 100-fold, 200-fold and 7 000-fold more sensitive than conventional visual AuNPs-based LFIA, respectively. In addition, the quantitative PT-LFIA and SERS-LFIA sensors worked well in spiked real samples with acceptable recoveries of 96.2 – 106.7% and 98.2 – 105.2%, respectively. This assay demonstrated that the developed multimodal LFIA had a great potential to be a powerful tool for accurate tracing hazardous analytes in complex samples.
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CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Xiaonan Duan,Jiabin Yin,Mengmeng Huang,Peixia Wang,Jisong Zhang
Halogenated aromatic anilines are series of crucial intermediates for the synthesis of pigments, medicines and pesticides in the fine chemistry. However, efficient inhibition of undesired dehalogenation is difficult to achieve in the commonly used batch reactors. Although employing continuous flow technology and modified catalysts could alleviate dehalogenation, obtaining high selectivity of halogenated aromatic anilines especially for brominated aromatic amines and iodine aromatic amines is still challenging. In this study, a continuous flow system based on micro-packed bed reactor was developed and a kinetic model of the hydrogenation of halogenated nitrobenzene was established. Kinetic parameters for the reductions of p -chloronitrobenzene, p -bromonitrobenzene and p -iodonitrobenzene were acquired and the kinetic model exhibited good fit for the transformation of each substance. Moreover, the accuracy of kinetic model was validated by the comparison with the values in literature. The obtained kinetic model offered helpful information for the process optimization of hydrogenation of halogenated nitroaromatics in continuous flow system.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Aiqun Kong,Menghui Liu,Houjun Zhang,Zifan Cao,Jinli Zhang,Wei Li,You Han,Yan Fu
Cyclohexanecarboxylic acid (CCA), an important chemical and pharmaceutical intermediate, is commonly produced from thermal catalytic hydrogenation of benzoic acid (BA) under high temperature and pressure. Herein, electrocatalytic hydrogenation (ECH) for highly selective conversion of BA into CCA using carbon fibers with different graphitization degree (carbon fiber paper (CFP), carbon fiber cloth (CFC)) supported commercial platinum carbon (Pt/C) electrode was reported for the first time without using external H 2 . Our experimental results show that, at room temperature and 1 atm, the BA conversion and the CCA selectivity are both as high as 100% in 0.05 M H 2 SO 4 over carbon fiber paper (CFP)-supported Pt/C (Pt/C/CFP). Meanwhile, Pt/C/CFP electrode still maintains outstanding stability after 10 reaction cycles. In situ Raman results and theoretical calculations reveal that the adsorption strength of BA over Pt/C/carbon fibers electrode varies with the graphitization degree of carbon fibers along with the applied potential. The superior ECH performance of the Pt/C/CFP is mainly attributed to the high dispersity of Pt/C catalysts on CFP as well as unique electronic interaction, which improved the adsorption and activation of BA. Typically, CFP with few defects can induce the accumulation of electrons around the Pt regions and enhance the electron-deficient aromatic adsorption thus improving the ECH performance of Pt/C/CFP, which is the opposite for CFC with more defects.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 4
·047507
·
IF 4.386
Li Su,Yarong Cheng,Jiaci Shi,Xuefeng Wang,Pengcheng Xu,Ying Chen,Yuan Zhang,Sen Zhang,Li Xinxin
Formaldehyde (FA) in food is harmful to human health, an effective detecting tool is highly desired especially for the on-site test. Herein, an amperometric aqueous FA sensor was fabricated by applying Pt–Ag core-shell nanoparticles as electrocatalyst. The well-characterized core-shell nanostructure exhibits high electro-catalytical activity for the detection of FA molecules in solution due to the synergistic effect of bimetallic Pt–Ag nanostructure. The proposed sensor exhibits high FA sensing performance, with a linear detection range from 1 to 100 μM and a limit of detection (LOD) down to 1.0 μM on the optimized conditions. Interferents coexisting in food samples were efficiently minimized by good selectivity. The Pt–Ag nanostructure-based FA sensor keeps catalytical activity for at least 30 d and shows good batch reproducibility. The proposed sensor was applied for the detection of FA in the food samples and satisfactory results were obtained, showing potential for the fast, simple, disposable, and cost-effective FA detecting method for food safety.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Xue-Yan Wu,Li-Yuan Zhu,Jie Sun,Kai-Yue Zhu,Xiao-Yong Miao,Meng-Yang Liu,Xue-Feng Zhao,Hong-Liang Lu
Pt nanoparticle (NP)-modified SnO2–ZnO (SnO2–ZnO–Pt) core–shell nanosheets (NSs) for hydrogen sulfide (H2S) gas sensing were successfully synthesized via atomic layer deposition, hydrothermal method, and magnetron sputtering. More importantly, the SnO2–ZnO–Pt NS sensing materials were synthesized in situ on microelectromechanical system (MEMS) devices, which are expected to be high-performance gas sensors with superior sensitivity, great selectivity, good reproducibility, and low power consumption. To be specific, the SnO2–ZnO–Pt NSs displayed a high sensitivity (Ra/Rg) of 30.43 and an excellent selectivity when detecting 5 ppm H2S at an operating temperature of 375 °C. Their rate of resistance change was 29.43, which was about 24 and 9 times those of the pristine SnO2 NS (∼1.25) and SnO2–ZnO core–shell NS (∼3.43) sensors, respectively. These substantially improved sensing properties could be mainly attributed to the formation of heterojunctions, catalytic sensitization effect, and increased specific surface area of Pt NP modification. Thus, the proposed SnO2–ZnO–Pt NS gas sensors demonstrate great potential as a high-performance sensing material for application in H2S gas sensors.
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CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Yu-Xuan Xiao,Jie Ying,Jiang-Bo Chen,Yuan Dong,Xiong Yang,Ge Tian,Jinsong Wu,Christoph Janiak,Kenneth I. Ozoemena,Xiao-Yu Yang
The heavy d-π effect is an important theoretical model for strong Pt–C interaction, and its enhancement is critical to the high-performance design of Pt/C electrocatalysts. Common chemical N-doping to the carbon support can provide possibilities for enhanced electrocatalysis but most often leads to random interaction with Pt nanoparticles (Pt-NPs) and uncontrollable tuning of the heavy d-π effect. Directional confinement of Pt-NPs within N-doped carbon to directly enhance the heavy d-π effect is therefore mostly preferred but rarely reported. Herein, confined ultrafine Pt-NPs in N-doped porous carbon fibers (Pt@NDPCF) were obtained by a combination method involving electrospinning, carbonization, and directional replacement. Such a synthetic strategy leads to highly dispersed, ultrafine Pt-NPs in hierarchically porous carbon fibers and a strong directional interaction of Pt with pyridinic N, which significantly enhances the heavy d-π effect, greatly facilitating electron transfer and optimizing Pt 5d orbitals. Based on these advances, Pt@NDPCF exhibited outstanding activity and superior durability in the hydrogen evolution reaction (HER), with 24 mV lower overpotential at 10 mA cm–2 and a much smaller activity loss after 10,000 cycles of durability tests in comparison with a commercial Pt/C catalyst. This work sheds new lights on the design of high-performance Pt-based nanomaterials toward HER or other practical applications.
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高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Linfang Lu,Yuelin Gu,Weiyi Guo,Fengyan Lu,Yunxia Li
The synthesis of ultrasmall-sized nanoparticles (NPs) has attracted serious attention in the past several years because of the largely increased surface-to-volume ratio of these NPs. Ligands are necessarily used to synthesize these NPs. However, the traditional ligands employed in the colloidal synthesis process would be strongly adsorbed on the surface of the metal NPs, leading to incomplete exposure of catalytically active sites. Here, we develop an efficient solid-state method to synthesize carbon-supported extrasmall ligand-free Pt nanoparticles (Pt SNPs/C) or Pd SNPs/C on a large scale (up to gram equivalent). The strong interfacial interaction between the modified carbon support and inorganometallic precursor is believed to successfully prepare this Pt SNPs/C catalyst. In particular, the fabricated Pt SNPs/C catalyst is ligand-free, which is carefully verified by different techniques (thermogravimetric analysis, X-ray photoelectron spectroscopy, and “electrochemical surface area (ECSA)” measurement). Because of the higher ECSA, Pt SNPs/C exhibits better catalytic activities toward methanol oxidation and hydrogen evolution than commercial Pt/C. By applying the catalyst as both the anode and cathode in a methanol-assisted water splitting system, the cell displays much better efficiency to produce highly valued hydrogen compared to that of commercial Pt/C components.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Mengjie Ma,Yi Zhang,Yujin Ji,Qi Shao,Kui Yin,Wenxiang Zhu,Junjun Yang,Fan Liao,Zhenglong Fan,Yang Liu,Youyong Li,Mingwang Shao,Zhenhui Kang
Poisoning species, such as methanol and air pollutants, degrade the electrocatalytic activity for oxygen reduction reaction (ORR). Here, via taking advantage of the varied electronic property of nano-silicon, a versatile strategy is reported for enhancing the catalytic activity and anti-poisoning ability toward ORR by decorating noble metal catalysts with the size-controlled silicon nanoclusters (DS). Consequently, DS-Pd exhibits the enhanced ORR performance with a large halfwave potential of 0.892 V and an onset potential of 1.010 V. More importantly, it also shows enhanced anti-poisoning performance in methanol, NaNO 2 and NaHSO 3 electrolytes, compared to those of commercial Pt/C and Pd/C catalysts. Mechanism studies reveal that the synergistic effect between Pd and more oxygen-philic and less poison-philic Si nanoclusters largely abbreviate the absorption of poisoning species on the active sites. This strategy also improves the methanol-tolerant performance of Pt based catalysts, providing a versatile strategy for the fabrication of methanol-tolerant ORR catalysts.
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