Molecular Catalysis
·
2024
·
IF 3.9
Hao Qin,Hui Wan,Guofeng Guan
Single atom catalysts have been recently reported as the efficient catalysts for hydroisomerization compared to the conventional nanoparticle catalyst. Despite the fascinating advantage in enhancing the metal activity or reducing the catalyst cost, the long-term stability of the single atom catalyst seemed not that satisfactory, especially when reacting under atmospheric pressure. Herein, Pt single atom catalysts were combined with Cu nanoparticles by different means to explore a new way to improve the catalytic performance. Cu nanoparticles were located away from Pt sites to form a binary catalyst, or acted as the support of Pt atoms to form a single atom alloy (SAA) catalyst. With the binary catalyst Pt 1 –0.1Cu@CS, the conversion of the n -heptane after time on stream of 50 h increased to 70.3 %, higher than Pt 1 @CS (47.3 %). Besides, excessive Cu nanoparticles in the binary catalyst were found rather harmful to the catalysis instead. However, the SAA catalyst Pt 1 Cu@SAPO-11 showed a poor activity in hydroisomerization compared to Pt 1 @CS, indicating that the alloy structure should go against the activation of reactant. The roles of Pt atoms and Cu nanoparticles in different catalysts were discussed in detail. The reaction mechanism of hydroisomerization was refined with the different functions of the dual metal sites. This work might be instructive for the design of single atom catalysts combined with metal nanoparticles.
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ACS Catalysis
·
2019
·
IF 12.221
Yan-Rong Liu,Xue Li,Wen-Min Liao,Ai-Ping Jia,Yue-Juan Wang,Meng-Fei Luo,Ji-Qing Lu
The Pt catalysts supported on hexagonal BN (Pt/BN) are highly active and stable for propane combustion, with the highest specific reaction rate of 92.3 μmol gPt–1 s–1 and turnover frequency of 0.037 s–1 obtained on a 0.2Pt/BN catalyst at 220 °C. The Pt oxide in the catalyst could be partially reduced to the metallic state by propane during the reaction, which is beneficial for the improvement of activity, indicating that metallic Pt might be the active sites. The highly dispersed Pt particles stabilized at the grain boundary of BN could be more easily reduced in the reaction than those on the surface and thus are more active. Moreover, kinetic investigation reveals that the apparent activation energy of the Pt species at the grain boundary (111.6 ± 8.0 kJ mol–1) is much lower than that on the surface (172.4 ± 16.5 kJ mol–1), suggesting different reaction pathways on these catalysts and the possible participation of the grain boundary of the BN support in the reaction.
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ANALYTICA CHIMICA ACTA
·
2016
·
IF 4.712
Liyuan Wang,Jiao Shan,Feng Feng,Zhanfang Ma
A novel electrochemical redox-active nanocomposite was synthesized by a one-pot method using N,N′-diphenyl-p-phenylediamine as monomer , and HAuCl 4 and K 2 PtCl 4 as co-oxidizing agents. The as-prepared poly(N,N′-diphenyl-p-phenylediamine)-Au/Pt exhibited admirable electrochemical redox activity at 0.15 V, excellent H 2 O 2 electrocatalytic ability and favorable electron transfer ability. Based on these, the evaluation of the composite as sensing substrate for label-free electrochemical immunosensing to the sensitive detection of carbohydrate antigen 199 was described. This technique proved to be a prospective detection tool with a wide liner range from 0.001 U mL −1 to 40 U mL −1 , and a low detection limit of 2.3 × 10 −4 U mL −1 (S/N = 3). In addition, this method was used for the analysis of human serum sample, and good agreement was obtained between the values and those of enzyme-linked immunosorbent assay, implying the potential application in clinical research. Importantly, the strategy of the present substrate could be extended to other polymer-based nanocomposites such as polypyrrole derivatives or polythiophene derivatives, and this could be of great significance for the electrochemical immunoassay .
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SURFACE REVIEW AND LETTERS
·
2015
·
IF 0.38
MINGSHU XIAO,YUHUA YAN,KAI FENG,YANPING TIAN,YUQING MIAO
A new electrochemical technique to detect hydrogen peroxide ( H 2 O 2 ) was developed. The Pt nanoparticles and Bi III were subsequently assembled on agmatine sulfate (AS) modified glassy carbon electrode (GCE) and the prepared GCE–AS- Pt – Bi III was characterized by scanning electron microscopy (SEM) with result showing that the flower-like nanostructure of Pt – Bi III was yielded. Compared with Pt nanoparticles, the flower-like nanostructure of Pt – Bi III greatly enhanced the electrocatalysis of GCE–AS- Pt – Bi III towards H 2 O 2 , which is ascribed to more Pt – OH obtained on GCE–AS- Pt – Bi III surface for the presence of Bi III . Based on its high electrocatalysis, GCE–AS- Pt – Bi III was used to determine the content of H 2 O 2 in the sample of sheet bean curd with standard addition method. Meantime, its electrocatalytic activity also was studied.
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ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Zizheng Fan,Dong Zhao,Qunshou Wang,Ling Chang,Liang Zhang,Junjie Yan,Haiyan Du,Mingyang Zheng,Wenxiang Wang,Wenli Pei
Pt-based high-entropy intermetallic (HEI) nanocatalysts have attracted widespread attention due to their promising catalytic performance. However, synthesis of HEI nanoparticles with fine size and highly ordered structure faces significant challenges. Herein, we employed Cu as a bridging element to successfully synthesize ultra-fine (5.23 nm), highly ordered Pt 4 FeCoNiCu-HEI nanoparticles. The moderate reduction potential of Cu facilitates uniform co-reduction, controlling nanoparticle growth. The low surface energy of Cu promotes its migration to the particle surface during high-temperature annealing, creating lattice vacancies that significantly lower the ordering energy barrier. The resulting nanocatalyst exhibits enhanced alkaline hydrogen evolution reaction (HER) performance, achieving low overpotentials of 15.8 mV and 96.8 mV at current densities of 10 mA cm -2 and 100 mA cm -2 , respectively – approximately half those of commercial Pt/C (36.2 mV and 206.2 mV). The nanocatalyst demonstrates outstanding stability, maintaining its performance after 10,000 CV cycles and 30 hours of chronopotentiometry testing. Density functional theory (DFT) calculations reveal that lattice distortion and multi-element doping synergistically lower the d-band center of Pt active sites, optimizing hydrogen adsorption free energy. Additionally, the transition metal constituents significantly reduce the energy barrier for the water dissociation step. This work presents a novel strategy for designing high-performance HEI nanocatalysts combining small size, high ordering, and optimized electronic structure. Download: Download high-res image (299KB) Download: Download full-size image
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ACS Applied Nano Materials
·
2025
·
IF 5.5
Hao Ren,Yi Cao,Tianjiao Ling,Junli Zhu,Jifang Xu,Minqi Sheng
Even though cobalt monophosphide (CoP) has been recognized as a prospective alternative to noble metal-based electrocatalysts in alkaline water splitting, further enhancement of the catalytic activity and durability of CoP in the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) requires precise manipulation of its nanoscale spatial architecture and surface electronic structure. Herein, tremella-like Pt, B-codoped CoP nanostructures were successfully anchored on carbon cloth (Pt–B–CoP/CC) through a successive process involving wet chemical deposition, surface Pt impregnation, and phosphorization. The resultant Pt–B–CoP/CC exhibits excellent catalytic activity for both HER and OER, primarily attributed to (i) high-density active sites, (ii) enhanced surface conductivity, and (iii) appropriately modulated electronic structure via Pt, B codoping. In addition, Pt–B–CoP/CC exhibits superaerophobicity, enabling the maintenance of efficient exposure of active sites during electrolysis. In an alkaline medium (1.0 M KOH), the required overpotentials are 52.53 (at −10 mA cm–2) for HER and 224.37 mV (at 10 mA cm–2) for OER, which outperform most of the reported transition metal-based bifunctional catalytic electrode materials. The constructed Pt–B–CoP/CC||Pt–B–CoP/CC cell requires an ultralow cell voltage of 1.51 V (1.74 V) to drive a current density of 10 mA cm–2 (100 mA cm–2). After 100 h of continuous electrolysis, the cell voltage increment is almost negligible at 10 mA cm–2, while at 100 mA cm–2 it increases by only 1.97%, demonstrating the tremendous durability of Pt–B–CoP/CC and its potential applicability in industrial-grade electrolyzers. This study provides inspiration for designing and synthesizing advanced multifunctional catalytic electrodes with high efficiency and long-term stability.
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DOI
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CARBON
·
2026
·
IF 12.7
Xinya Gao,Qiaoling Li,Fang Liu,Shiying Zhang,Frank Ko,Hongqiang Wang,Zhongfu Li,Jiao Li
We present a single-step approach for producing ultra-microporous carbon membranes from lignin that eliminates spontaneous combustion during carbonization. A CO 2 -assisted electrospinning converts in situ NaOH→Na 2 CO 3 , enabling high-temperature self-activation without corrosive external agents. DFT further rationalizes CO-facilitated Na desorption, explaining the combustion-free carbonization. The resulting carbon membranes possess ultra-high surface area (2443 m 2 ·g -1 ) and narrowly distributed ultra-micropores (∼0.5 nm). At ultra-low Pt loadings (0.01 wt%), aberration-corrected HAADF-STEM and CO-pulse chemisorption reveal near single-atom dispersion (∼0.57 nm). The MC-Pt 0.01 (0.01 wt% Pt/microporous carbon) catalyst achieves 47.4% HCHO degradation at room temperature (70 ppm, 2 h, static) and 965 min fully penetrated with 262.5 mg·g -1 capacity (12 ppm, GHSV = 4000 L·g cat -1 ·h -1 ). Mechanistic analyses (EPR, O 2 -TPD, in situ DRIFTS) support a dual-site pathway, wherein vacancy-enriched ultra-micropores chemisorb HCHO, while atomically dispersed Pt activates O 2 to generate •O 2 - , driving complete mineralization to CO 2 . This strategy integrates waste-derived carbons with low-precious-metal catalysis, offering strong potential for sustainable indoor air purification and environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 12.5
Yani Dong,Li Chen,Jiaxin Liu,Guangmin Ren,Tuo Guo,Qingjie Guo
Photocatalytic nitrogen reduction reaction (PNRR) is an important tool for advancing carbon neutrality. However, effective N 2 adsorption and activation, and the subsequent dissociation of water, remain major challenges in the PNRR. In this work, FeVO 4 -based catalysts co-modified with Pt nanoclusters (NCs) and single atoms (SAs) (Pt/FeVO 4 ) are synthesized and applied in the PNRR. The synthesized Pt/FeVO 4 catalyst achieves a NH 3 production rate of 35.14 μmol·g −1 ·h −1 , 3.2 times higher than that of the original FeVO 4 , and the photocatalytic nitrogen fixation performance remains at a high level of 80% after four cycles. Density functional theory (DFT) calculations and various characterization experiments results show that the Pt NCs in the Pt/FeVO 4 catalysts can effectively promote the adsorption and dissociation of water, and the active hydrogen (*H) generated from the dissociation of water can migrate to the neighboring Pt SAs through the spillover effect. The local electron concentration around Fe is altered by the Pt SAs, which enables the activation and hydrogenation of N 2 , and thus enhances the efficiency of PNRR. This research emphasizes the essential effects of the dual active sites of NCs and SAs with hydrogen spillover in PNRR, which provides novel concepts for the design of highly efficient catalysts.
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CERAMICS INTERNATIONAL
·
2026
·
IF 5.6
Miao Yuan,Dashi Fu,Yaqi Wang,Chengwu Li,Guohui Zhu,Dingding Xu,Weiquan Shao,Yanqiang Li,Wanneng Ye,Yongcheng Zhang
Transparent piezoelectric ceramics, due to their ability to possess both piezoelectricity and light transmittance, have extensive applications in devices such as transparent sensors and transparent transducers. Generally, constructing ferroelectric domains with strong ferroelectricity and long-range order can yield a large piezoelectric coefficient. However, ferroelectric domain structures cause light scattering at the domain walls, thereby reducing the material's optical transmittance. Consequently, achieving both high optical transparency and a large piezoelectric performance simultaneously in piezoelectric ceramics presents a significant challenge. To address this challenge, La, Pr, Nd, Sm, Eu co-doped (1- x ) Pb(Mg 1/3 Nb 2/3 )O 3 - x PbTiO 3 (PMN-PT) transparent piezoelectric ceramics were prepared in this study based on a high-entropy strategy. Benefiting from the cocktail effect and lattice distortion effect of the high-entropy strategy, the largest piezoelectric performance d 33 of 1476 pC/N, along with a 60% linear transmittance and the highest linear transmittance up to 67% at 900 nm, along with high piezoelectric performance of 1334 pC/N were achieved. The influence of phase structure and ferroelectric domain structure on its optical, piezoelectric, dielectric, and ferroelectric properties was studied. The high-entropy transparent piezoelectric ceramics show enormous application potential in multifunctional photo-acoustic-electric coupling devices.
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JOURNAL OF MATERIALS CHEMISTRY
·
2012
·Vol. 22
·期 37
·19718-19725
·
IF 5.968
Xiao Zhao,Jianbing Zhu,Liang Liang,Jianhui Liao,Changpeng Liu,Wei Xing
The development of advanced support materials displays the potential for both reducing the cost and simultaneously increasing the activity of catalysts. In the current work, a novel N-doped carbon coated hydrophilic titanium dioxide (TiO2@N-doped C) nano-composite, constructed by the procedure of an in situ polymerization and subsequent pyrolysis, was utilized to support Pt nano-crystals for the methanol oxidation reaction (MOR). The as-prepared Pt/TiO2@N-doped C catalyst generated 1.74-fold higher activity, 2.08-fold higher stability and much better resistance to CO poisoning than a commercial state-of-the-art Pt/C catalyst. The enhanced catalytic performance was ascribed to the improved CO tolerance and the catalyst–support interaction due to the utilization of the TiO2@N-doped C nano-composite, which not only provides rich active –OH groups to promote CO oxidation via the bifunctional mechanism, but also modifies the electronic structure of the Pt NPs to improve the intrinsic kinetics of MOR. The as-developed TiO2@N-doped C nano-composite is a highly promising catalyst support material for use in fuel cell technology.
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ACS Catalysis
·
2023
·
IF 12.9
Xiaolong Liu,Yang Zou,Xue Li,Tieyao Xu,Wanglai Cen,Bin Li,Tingyu Zhu
Bimetallic catalysts Pt–M/Ti were prepared by introducing various dopants (M = Mn, Fe, Co, Cu, Ce, Mo) into Pt/Ti with ultralow loadings (0.5 wt % M) and compared in CO oxidation in the presence of H2O and SO2. Among these catalysts, Pt–0.5Mn/Ti contributed the highest oxidation efficiency and strongest sulfur resistance. Further improvement of Mn contents led to the decrease of CO conversion. It was indicated that the introduction of appropriate Mn species enhanced the active oxygen supplying ability of the catalyst, thus improving the reaction activity. The CO oxidation performance of the catalyst was improved through the reaction between *OH from H2O dissociation and CO. The deposition of S on the Pt–0.5Mn/Ti surface did not increase with time extension. Theoretical calculation results revealed that cleavage of S–O–Mn species could be facilitated by Pt, and the SO2 adsorption energy calculations demonstrated that SO2 was more easily adsorbed on Pt/Ti than Pt–0.5Mn/Ti, which was very consistent with its sulfur resistance. In situ DRIFT studies at 260 °C revealed that the introduction of SO2 onto Pt–0.5Mn/Ti showed little change for CO adsorption on different Pt species, while Pt/Ti showed an apparent decrease of Pt0–CO. 18O isotopic experiments in the presence of H218O and SO2 were systematically designed to accurately quantify the CO2 composition including C16O16O, C16O18O, and C18O18O. Accordingly, the reaction mechanism for Pt–0.5Mn/Ti catalyzed CO oxidation consisting of four pathways was proposed.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Weizhen Xie,Yue Tang,Jiacheng Li,Yaqi Shi,Shigang Su,Yong Sun,Lu Lin,Xing Tang
The aqueous-phase hydrogenation of concentrated 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) is a crucial transformation for sustainable chemical production. However, this process is often limited by sluggish H 2 activation at low temperatures and poor selectivity arising from over-hydrogenation. Here, we develop a Pt catalyst supported on oxygen-deficient manganese oxide (Pt/MnO x –O v ), featuring finely dispersed Pt/PtO 2 domains in conjunction with abundant Pt–O–Mn interfacial ensembles. Under mild aqueous conditions (30–60 °C), the catalyst efficiently converts HMF at concentrations up to 40 wt%, delivering a BHMF yield of 90.9 %. In addition, continuous-flow operation at 30 °C sustains BHMF yields above 90 % over a cumulative operation time of 80 h, thereby demonstrating promising potential for industrial application. Mechanistic studies suggest that hydrogen is initially activated on Pt nanoparticles and subsequently undergoes in situ spillover, migrating across the Pt/PtO 2 heterostructure toward adjacent Pt–O–Mn interfacial sites. At these interfacial regions, the asymmetric electronic distribution, induced by nearby oxygen vacancies, facilitates the formation of polarized H δ+ –H δ- species. These reactive hydrogen species, together with the preferential adsorption of the carbonyl group, enable selective hydrogenation while suppressing undesired side reactions. This study demonstrates that tailoring interfacial structures is an effective strategy for improving catalytic performance in biomass upgrading.
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