ENERGY
·
2025
·
IF 9.4
Qingqing Liu,Huiyuan Liu,Weiqi Zhang,Qian Xu,Lindiwe Khotseng,Sivakumar Pasupathi,Huaneng Su
The performance of high-temperature proton exchange membrane fuel cells (HT-PEMFCs) is severely limited by the poisoning effect and low oxygen solubility of the phosphoric acid (PA) electrolyte. To address this, we report an innovative catalyst architecture consisting of one-dimensional hollow PtNi nanochains coated with a functional ionic liquid (IL), termed PtNi@IL/C. This design creates a multifunctional interface that demonstrates exceptional PA tolerance, achieving an oxygen reduction reaction (ORR) half-wave potential of 0.840 V in a PA-containing electrolyte, which is 90 mV higher than commercial Pt/C. The IL coating synergistically enhances performance by suppressing PA adsorption on Pt active sites while simultaneously boosting O 2 mass transport through its high oxygen solubility, and providing a highly efficient proton conduction pathway. As a result, a membrane electrode assembly utilizing the PtNi@IL/C catalyst achieves a high peak power density of 521 mW cm −2 at 150 °C. Furthermore, the catalyst exhibits outstanding durability, with a negligible 4 mV activity loss after 5000 electrochemical cycles and only a 2 % power density decay in single-cell tests, significantly outperforming the 14.3 % decay of Pt/C. This stability is attributed to the IL mechanically reinforcing the porous nanochain structure, preventing degradation. This work presents a powerful catalyst-interface engineering strategy for developing next-generation, high-performance fuel cells.
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Yi-Fan Xue,Fei Zhao,Jie Feng,Wen-Ying Li
In hydrofining processes, the competitive interactions among sulfur-containing compounds, aromatic hydrocarbons, and nitrogen-containing intermediates fundamentally govern catalytic performance. Nevertheless, the complex kinetic relationships within hydrodenitrogenation (HDN) systems have remained unclear and insufficiently investigated. This research comprehensively and systematically examined the competitive reaction kinetics of naphthalene (an aromatic model) and dibenzothiophene (a sulfur-based model) during the HDN of 1,2,3,4 - tetrahydroquinoline over Pt-based catalysts. Through systematic analysis of conversion rates and product distributions across various reaction conditions, it demonstrated that both dibenzothiophene and naphthalene exert distinct inhibitory effects on HDN through mechanistically differentiated pathways. Quantitative evaluation revealed a pronounced temperature dependence in mitigating these inhibitory effects, whereas pressure variations exhibited negligible influence. These findings collectively demonstrate that surface adsorption competition, rather than hydrogen availability, dictates the reaction kinetics. Rigorous kinetic calculations and rate constant fittings identified the hydrogenation of 1,2,3,4-tetrahydroquinoline to decahydroquinoline as the rate-limiting step susceptible to competitive inhibition. This phenomenon predominantly arises from the tripartite competitive adsorption among naphthalene, dibenzothiophene, and 1,2,3,4-tetrahydroquinoline at catalytic active sites, as corroborated by theoretical adsorption energy calculations. Notably, the two inhibitors manifest divergent interaction mechanisms: H + ions generated during H 2 S formation in dibenzothiophene desulfurization facilitate C–N bond cleavage, whereas naphthalene directly suppresses this critical step. Furthermore, atomic-layer-deposited TiO 2 on Pt/Al 2 O 3 engineered the catalyst surface through three synergistic effects: enhanced nitrogen adsorption capacity, optimized hydrogen spillover pathways, and generation of additional C–N bond cleavage sites. This multi-effect strategy effectively reduces the negative impacts of competitive adsorption, emphasizing the crucial role of competitive reaction kinetics in designing sulfur/aromatic-resistant HDN catalysts.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 3
·1686-1694
·
IF 3.591
Kezhong Wu,Pengyuan Fu,Bei Ruan,Mengmeng Wu,Mingxing Wu,Ruitao Wu
Replacing the expensive Pt catalyst of counter electrodes (CEs) with a low-cost Pt-free catalyst has been regarded as one of the crucial steps for cost effectiveness of dye-sensitized solar cells (DSSCs). Herein, MnWO4 as a binary mixed oxide (MnO–WO3) has been prepared with (NH4)10H2(W2O7)6·xH2O and Mn(NO3)2·4H2O via a facile hydrothermal method. DSSCs using MnWO4 CEs show power conversion efficiency (PCE) of 4.93%. To improve the catalytic activity of MnWO4 CEs further, three proportions of MnWO4@AC mixed oxide composite catalysts have been fabricated via simple physical mixing MnWO4 with activated carbon (AC) by ball-milling. Moreover, the DSSCs with the MnWO4@AC composites CEs generate high PCE of 6.50, 6.45 and 6.12%, respectively, from MnWO4 : AC mass ratios of 1 : 2, 1 : 1 and 2 : 1 for the regeneration of traditional iodide/triiodide (I3−/I−) redox couples, which were superior to the pristine MnWO4, Pt- and AC-based counterpart 4.93%, 4.54% and 2.10% CEs under the same test conditions and method. The favorable performances make MnWO4@AC composites act as a new resource of electro-catalytic Pt-free materials for high-performance CEs in the encapsulation of DSSCs.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2017
·
IF 2.536
Weiguo Wang,Yake Zou,Jinwu Yan,Jing Liu,Huixiong Chen,Shan Li,Lei Zhang
In this paper, an ultrasensitive colorimetric biosensor for human chorionic gonadotrophin (hCG) detection was designed from bottom-up method based on the dual catalysis of the horseradish peroxidase (HRP) and Au@Pt nanoparticles (NPs) relative to H 2 O 2 -TEM system. HRP and monoclonal mouse anti-hCG antibody (β-submit, mAb 1 ) were co-immobilized onto the Au@Pt NP surface to improve catalytic efficiency and specificity, which formed a dual functionalized Au@Pt-HRP probe with the mean size of 42.8 nm (D 50 ). The colorimetric immunoassay was developed for the hCG detection, and the Au@Pt-HRP probe featured a higher sensitivity in the concentration range of 0.4–12.8 IU L − 1 with a low limit of detection (LOD) of 0.1 IU L − 1 compared with the LODs of 0.8 IU L − 1 for BA-ELISA and of 2.0 IU L − 1 for Au@Pt, which indicated that the Au@Pt-HRP probe possessed higher catalytic efficiency with 2.8-fold increase over Au@Pt and 33.8-fold increase over HRP. Also, the Au@Pt-HRP probe exhibited good precision and reproducibility, high specificity and acceptable accuracy with CV being less than 15%. The dual functionalized Au@Pt-HRP probe as a type of signal amplified method was firstly applied in the colorimetric immunoassay for the hCG detection.
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CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Yi Wang,Jialiang Chen,Lan Wang,Hanqin Weng,Zhihao Wu,Limin Jiao,Yusa Muroya,Shinichi Yamashita,Sheng Cheng,Fuhai Li,Hongbing Chen,Wei Huang,Mingzhang Lin
The large-scale synthesis and the stabilization of noble metal nanocatalysts with ultrasmall sizes are crucial to their practical application. Herein, Pd, Au, and Pt nanoparticles (NPs) are in situ embedded on boron nitride nanosheets (BNNSs) via the reduction of precursor salts induced by 60 Co γ-irradiation, which is a mature technique widely used in industry. The reduction mechanism was elucidated by pulse radiolysis experiments. In comparison with other BN substrates like hexagonal BN ( h -BN), BNNSs had not only large surface area of 263 m 2 g −1 , but also abundant hydroxyl groups produced during the sonicated exfoliation, resulting in ultrasmall sizes, large loading amounts, and uniform distribution of the anchored NPs. The particle sizes of the loaded Pd, Au, and Pt NPs were measured to be 2.9, 3.1, and 3.0 nm, respectively. As a consequence, in the model reaction of 2-nitroaniline reduction, the Pd-, Au- and Pt-BNNSs composite nanocatalysts showed much higher catalytic activities than those composites loading the corresponding NPs on other BN substrates. Particularly, most of the 2-nitroaniline could be reduced within merely 40 s when using Pd-BNNSs as catalysts, performing a rate constant of 1.1 × 10 −1 s −1 . The number of hydroxyl groups on BNNSs support as well as the catalytic performance of the corresponding NPs-loaded BNNSs composites could be improved by extending the sonicated exfoliation time, because more NPs were loaded and the hydroxyl groups were also proved to play an important role in enhancing the catalytic activity. Moreover, Pd-BNNSs catalysts still displayed prominent activity even after five cycles owing to the high stability of BNNSs and their strong affinity for PdNPs. This work not only demonstrates BNNSs as ideal supports to load noble metal NPs for catalysis, but also reveals the feasibility to synthesize and in situ embed ultrasmall noble metal NPs on BNNSs via γ-irradiation.
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Nanoscale Research Letters
·
2013
·Vol. 8
·期 1
·1-8
·
IF 2.524
Jamal Ruxangul,Xu Feng,Shao Weiwei,Abdiryim Tursun
The solid-state method was applied for synthesizing polyaniline (PANI)/noble metal hybrid materials with the presence of HAuCl 4 ·4H 2 O or H 2 PtCl 6 ·6H 2 O in the reaction medium. The structure, morphology, and electrochemical activity of the composites were characterized by Fourier transform infrared (FTIR) spectra, UV-visible (vis) absorption spectra, energy dispersive spectrum (EDS), X-ray powder diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), and cyclic voltammetry. The results from FTIR and UV-vis spectra showed that the oxidation degree and doping level of the PANI in composites can be influenced by HAuCl 4 ·4H 2 O and H 2 PtCl 6 ·6H 2 O. The EDS data demonstrated that the composites contain a certain amount of Au (or Pt) element. XRD analysis indicated the presence of crystalline-state Au particles in PANI matrix prepared from the presence of HAuCl 4 ·4H 2 O and revealed that the H 2 PtCl 6 ·6H 2 O cannot be converted into metal Pt. The TEM and SEM images implied that the Au particles did exist in the polymer matrix with the size of about 20 nm. The enzymeless H 2 O 2 sensor constructed with PANI/Au composite from the presence of HAuCl 4 ·4H 2 O showed a short response time (within 5 s) and displayed an excellent performance in wide linear range.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Jingyu Wang,Min Xu,Jianquan Zhao,Huaifang Fang,Qingzhu Huang,Weiping Xiao,Tao Li,Deli Wang
The activity and stability of Pt electrocatalysts are crucial issues for energy conversion systems involving oxygen reduction reaction (ORR). In this work, the ultrafine Pt nanoparticles were in situ reduced by the photogenerated electrons on TiO 2 surface so that most of them selectively anchored around the TiO 2 nanocrystals. The presence of well-dispersed TiO 2 on carbon surface strengthened the metal-support interaction, giving rise to the improved ORR catalytic activity with ∼49 mV positive shift of half-wave potential as compared to commercial 20 wt% Pt/C. More importantly, the Pt/TiO 2 -C catalysts exhibited a more durable performance after 10,000 cycles in terms of the decrease in electrochemical surface area (0.8%) and mass activity (0.9%), much lower than those of Pt/C (10.2% and 33.3%). The high-temperature durability test also revealed a much higher retention of ORR activity. The results demonstrated that anchoring Pt on well-dispersed TiO 2 -decorated carbon would be an effective strategy to enhance the ORR performance by strong metal-support interaction, which facilitated the electron transfer during catalytic reactions as well as prevented Pt aggregation during durability test.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Chunjie Li,You Xu,Dandan Yang,Xiaoqian Qian,Xingjie Chai,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
The exploration of highly efficient catalysts for electrochemical hydrogen and oxygen production via water splitting is very significant for providing affordable clean energy and reducing the reliance on conventional fossil fuels. Herein, we develop an efficient method to boost the electrocatalytic performance of Pt mesoporous nanoparticles (Pt MNs) for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) by a facile Ni, P co-incorporation strategy. The co-incorporation of Ni and P atoms in a Pt crystal structure can effectively modify its electronic structure, which contributes to the superior catalytic ability toward HER. We also demonstrate that the as-fabricated PtNiP MNs could occur surface partial oxidation under oxidizing potentials to in situ form OER electroactive oxides/hydroxides species. The unique mesoporous structure and metal–nonmetal ternary alloyed composition make the PtNiP MNs a promising HER–OER bifunctional electrocatalyst for overall water splitting in alkaline media.
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RSC Advances
·
2022
·Vol. 13
·期 1
·448-455
·
IF 4.036
Kyong-Sik Ju,In-Ho Jang,Yong-A. Choe,Song-Chun Ri,Hyon-Tae Pak,Su-Ok Hong
A carbon supported Pt–Cu electrocatalyst was synthesized by the microwave-polyol method following acid-treatment and physically characterized by different techniques including X-ray diffraction (XRD) and transmission electron microscopy (TEM). Both potentiodynamic and potentiostatic measurements with pinhole on-line electrochemical mass spectrometry were carried out to study the electrocatalytic activity and reaction intermediates of Pt/C and Pt–Cu/C electrocatalysts during the ethanol oxidation reaction. The results of potentiodynamic and potentiostatic measurements showed that the Pt–Cu/C electrocatalyst has higher ethanol oxidation efficiency and incomplete ethanol oxidation to acetaldehyde and acetic acid prevails under the given conditions. After calibration of the m/z = 44 mass signal, the CO2 current efficiencies on Pt/C and PtCu-3/C were ∼7% and ∼12%, respectively, which reveal that the presence of copper enhances the complete ethanol oxidation to CO2.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2015
·
IF 2.495
Xiaoqin Wang,Yong Zhang,Qiangqiang Xu,Jinxin Xu,Bohua Wu,Min Gong,Jia Chu,Shanxin Xiong
A low-cost quasi-solid dye-sensitized solar cell (DSSC) with a photoelectric conversion efficiency of 1.79% was assembled using PVDF-based gel electrolyte plasticized by PC–EC and electrodeposited Pt counter electrodes. Its morphology, chemical structure, electrochemical and photoelectric properties were examined by SEM, FTIR, EIS and I – V tests, respectively. The results showed that PC–EC plasticized gel electrolyte can greatly prevent the α-phase formation of PVDF, and had the loose structure & many interpenetrating holes due to the effective intercalation of PC & EC into PVDF chains through their dipole interaction. It made the migration or diffusion of iodide ions to electrodes easier. Furthermore, its conductivity was increased to 2.34 mS/cm from 1.00 mS/cm of unplasticized gel electrolyte. V oc , J sc , FF & η values of DSSC plasticized by PC–EC were all enhanced. Compared with Pt electrode obtained by thermal decomposition, electrodeposited Pt electrode had the lower charge-transfer resistance and the better contact with gel electrolyte in quasi-solid DSSC due to its orderly grain arrangement, more even, denser and larger active surface. Meanwhile, its process also had little influence on ITO sheet resistance. Thus, its quasi-solid DSSC has the higher photoelectric conversion efficiency.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2017
·
IF 4.233
Yan Gao,Yiwei Zhang,Yuming Zhou,Chao Zhang,Hongxing Zhang,Shuo Zhao,Jiasheng Fang,Mengqiu Huang,Xiaoli Sheng
In this work, we report a feasible approach to synthesize a ternary nanocomposites , Pt/lanthanum doped mesoporous zirconium oxide (Pt/La 2 O 3 -ZrO 2 ), via an effective two-step method. Ordered mesoporous La 2 O 3 -ZrO 2 composites were firstly fabricated with mesoporous silica KIT-6 as a hard template. Subsequently, uniform Pt nanoparticles encapsulated by 4 hydroxyl-terminated poly (amidoamine) (G4-OH PAMAM) dendrimers were deposited on the La 2 O 3 -ZrO 2 composites. The as-prepared samples were characterized by transmission electron microscope (TEM), N 2 adsorption–desorption isotherm analysis, energy dispersion X-ray analysis (EDX), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and temperature programmed reduction (H 2 -TPR). The average size of PtDENs was found to be 1.48 nm in diameter. Furthermore, the introduction of La could improve the structure of the supports which was confirmed by XRD and H 2 -TPR analysis. The reduction of p-nitrophenol to p-aminophenol by NaBH 4 was utilized to evaluate the catalytic performances of catalysts. Results indicated that the Pt/La 2 O 3 -ZrO 2 catalyst calcined in nitrogen at 550 °C exhibited the highest catalytic performance and still kept the high catalytic activity even after six cycles. This phenomenon suggests that synergistic effect among Pt-Zr-La could enhance the catalytic efficiency. Finally, reaction mechanism was proposed for the reduction of p-nitrophenol.
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Changhui Liang,Yuxin Zhang,Jun Shen,Xiaoqiang Zhang,Huixiang Li,Songhai Xie,Yongxin Li,Z. Conrad Zhang
The development of bifunctional electrocatalysts with high efficiency for overall water splitting is still a challenging task. In this work, we introduce a novel one-step synthesis method for Pt/NiFe layered double hydroxide (LDH) on an iron-nickel foam (INF) substrate under mild conditions. This method eliminates the need for additional Ni or Fe ions and facilitates in-situ etching and growth processes under mild conditions, resulting in a higher active surface area, well-dispersed low-loading Pt nanoparticles, and a self-supported electrode without binders. These features collectively enhance electron transfer and catalytic activity for both HER and OER. The Pt/NiFe LDH/INF exhibits remarkable water splitting performance, requiring a cell voltage of only 1.44 V at10 mA cm −2 when used as both anode and cathode. Additionally, it remains stable at 20 mA cm −2 for at least 16 h. The exceptional water splitting activity of Pt/NiFe LDH/INF in alkaline solution can be attributed to the synergistic effects of Pt and NiFe LDH, which improve the hydrogen evolution reaction and oxygen evolution reaction efficiencies. The results provide valuable insights into designing bifunctional electrocatalysts with low Pt loading for optimal water splitting performance at low operating cost.
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