MICROCHIMICA ACTA
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2026
·Vol. 193
·期 10
·679
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IF 5.4
Wu Siying,Du Tianmei,Ma Mengyun,Pu Fang,Zhang Yanli,Men Xue,Wang Hongbin,Yang Wenrong,Pang Pengfei
The development of a novel molecularly imprinted electrochemical sensor for the sensitive and selective detection of bisphenol A (BPA) is reported, based on a nanocomposite comprising dendritic Pt–Pd bimetallic nanoparticles and graphitic carbon nitride (Pt–Pd NPs/g-C 3 N 4 ). The molecularly imprinted polymer (MIP) was fabricated via electrochemical polymerization on Pt–Pd NPs/g-C 3 N 4 nanocomposite modified screen-printed electrode (Pt–Pd NPs/g-C 3 N 4 /SPE) surface. The synergistic integration of porous Pt–Pd NPs and ultrathin g-C 3 N 4 nanosheets provides a larger effective surface and enhances catalytic activity for BPA determination. The MIP film was fabricated via cyclic voltammetry on the modified electrode, employing BPA as the template molecule and pyrrole as the functional monomer. Following template removal, the resulting molecularly imprinted cavities within the MIP demonstrated high specificity for BPA recognition. The fabricated MIP-based electrochemical sensor exhibited an excellent linear response and high sensitivity for BPA detection over a broad concentration range of 2–100 ng/mL, achieving a limit of detection (LOD) of 0.2 ng/mL (3 σ/S ) and a limit of quantification (LOQ) of 0.6 ng/mL. The MIP-based sensor exhibits outstanding specificity, reproducibility, and operational stability, thereby providing a versatile platform for rapid and ultrasensitive BPA detection—a critical capability for ensuring environmental safety and protecting public health. Graphical
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MICROCHEMICAL JOURNAL
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2026
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IF 5.2
Faman Lin,Jiaqi Geng,Yanxin Lv,Zhitan Huang,Daniel Scherman,Shuhai He,Hongji Li,Tingting Sun,Wei Sun
Pt@COOH-MWCNT/PVA/AM hydrogel is synthesized by in situ gelation method. • Hydrogel modified electrode is used to sensitive electrochemical analysis of BPA. • Good properties of conductivity, antibacterial and salt-resistant are realized. • The sensor has a wide range of 0.05–1000.00 μM and a low LOD of 0.045 μM. Bisphenol A (BPA), which is extensively employed in plastics and food-contact products, poses serious hazards to the ecological environment and human health because of its endocrine disruptor property. Owing to its wide usage and environmental persistence, sensitive, selective and rapid BPA detection is urgently required, particularly in seawater. In this work, a conductive hydrogel prepared by anchoring Pt nanoparticles (NPs) onto carboxyl-functionalized multi-walled carbon nanotubes (COOH-MWCNT) was used to modify a glassy carbon electrode (GCE) for BPA electrochemical detection. The morphology and structure of the resulting composite were characterized, which revealed a dense, three-dimensional porous conductive network with fast electron transport ability and good mechanical stability. The incorporation of Pt@COOH-MWCNT significantly improved both the electrical conductivity and the electrocatalytic oxidation performance toward BPA. The fabrication and electrochemical detection parameters were optimized. Under optimal conditions (0.1 M phosphate buffer solution, pH 6.0), the sensor exhibits a BPA linear response range of 0.05–1000.00 μM with a detection limit of 0.045 μM, along with superior anti-interference, good stability, reproducibility (RSD = 0.9%), excellent salt tolerance, and antibacterial activity. When applied to real seawater samples, the recoveries were ranged from 97.50% to 106.00% with a relative standard deviation below 3.5%, confirming the sensor's favorable accuracy and reliability. The proposed sensor integrates robust structural integrity, enhanced conductivity, high catalytic activity, cost-effectiveness, and antibacterial performance, which offers a new strategy for on-site rapid monitoring of BPA in seawater environments with great application potential. The detection of bisphenol A (BPA) in seawater remains challenging due to complex matrices and the lack of simple, low-cost sensing platforms, as conventional electrochemical sensors often involve tedious fabrication or suffer from limited performance. Herein, a Pt@COOH-MWCNT/PVA/AM conductive hydrogel is fabricated via a straightforward in situ gelation strategy, providing a facile and cost-effective approach. Exploiting the high conductivity of COOH-MWCNT, the electrocatalytic activity of Pt nanoparticles, and the porosity, antibacterial property, and salt tolerance of the PVA/AM matrix, the constructed sensor achieves sensitive BPA detection over a wide linear range (0.05–1000 μM) with a low detection limit (0.045 μM), along with good reproducibility, anti-interference capability, and stability. Satisfactory recoveries (97.50%–106.00%) obtained in real seawater samples confirm its analytical reliability. This work offers a promising strategy for developing robust, low-cost electrochemical sensors suitable for on-site monitoring of BPA in complex marine environments. Download: Download high-res image (144KB) Download: Download full-size image
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Jing Jiang,Jiayi Zhang,Baihao Wu,Sheng Tu
The regulation of the metal-support interaction in heterogeneous catalysts can promote the activation of reactants, which is beneficial for the hydrolytic dehydrogenation reaction. Herein, the hydrolytic dehydrogenation of dimethylamine borane (DMAB) is systematically studied on the oxygen vacancy (O v ) enriched Pt-Co 3 O 4 heterogeneous catalyst with the metal-support interaction. It is found that the metallic Pt site facilitates the adsorption of DMAB molecules and the O v on Co 3 O 4 support as an electron-rich center cooperates with the adjacent Pt site to dissociate water molecules. The in situ Raman and attenuated total reflectance (ATR)-Fourier transform infrared (FTIR) spectroscopy reveal the effective activation and cleavage of the O-H in water and the B-H in DMAB over the Pt-Co 3 O 4 catalyst. The optimal Pt-Co 3 O 4 catalyst exhibits the extraordinary activity for the catalytic hydrolysis of DMAB at 303 K, delivering a high specific hydrogen generation rate (64063 mL min −1 g pt −1 ) and a competitive turnover frequency (TOF, 23880 mol H2 mol Pt −1 h −1 ). This performance outperforms most of the reported heterogeneous catalysts for DMAB dehydrogenation . More importantly, the Pt-Co 3 O 4 catalyst achieves the desirable on-demand hydrogen production by using special chemical switches. This finding provides the fundamental understanding of metal-oxide systems with the collaborative interfacial catalysis for boosting DMAB dehydrogenation .
研究领域:
催化化学
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纳米材料科学
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能源化学
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表面科学
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多相催化
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氢能存储与释放
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ELECTROCHIMICA ACTA
·
2023
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IF 6.6
Jiarun Cheng,Chaojie Lyu,Gang Dong,Yongqiang Liu,Yue Hu,Bin Han,Dongsheng Geng,Dongjie Zhao
Highly efficient and stable Pt-based electrocatalysts have broad application prospects in fuel cells, among which, Pt loading accompanied with particle size, interparticle distance (ipd), and interaction with support are identified as key contributors for high activity and selectivity. Herein, we have developed the nitrogen-doped graphite-like carbon sheets supporting low-Pt loading (Pt@N-GC) with uniform size and controllable ipd, and disentangled the main effect of ipd on oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) activity. The optimal 5.0 wt% low-Pt loading results in more abundant Pt sites and lower ipd, which leads to the higher surface reactivity by proximity effect , and 2e − pathway can be hindered by strongly resorbing and reducing H 2 O 2 to promote 4e − pathway towards ORR . Simultaneously, the 5.0 wt% Pt@N-GC can effectively improve the MOR activity, enhance the adsorption of -OH group under the appropriate ipd, so as to promote the instantaneous oxidation of CO and enhance the tolerance, and accelerate the oxidative dehydrogenation of methanol. Benefiting by the synergistic effect of Pt nanoparticles and N-GC support, all Pt@N-GCs exhibit bifunctional electrocatalytic activity and durability. We believe the gained trade-off of the loading and proximity effect of Pt, and its influence on catalytic activity and selectivity contributes to design more promising low-Pt loading bifunctional catalysts for fuel cell.
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FUEL
·
2023
·
IF 7.4
Fukun Bi,Shuting Ma,Bin Gao,Yang Yang,Lexun Wang,Fuhao Fei,Jingcheng Xu,Yuandong Huang,Minghong Wu,Xiaodong Zhang
Herein, Pd and Pt-catalysts loaded on non-oxide support (g-C 3 N 4 ) were prepared and compared for CO and toluene co-oxidation, and Pt/C 3 N 4 presented excellent catalytic performance. A series of characterizations including TEM, H 2 -TPR, O 2 -TPR and XPS etc., indicated that Pt/C 3 N 4 exhibited the smaller Pt NPs, better low temperature reduction ability, more active oxygen species and positive charged Pt species, which could account for its better catalytic performance. Additionally, DFT calculations further confirmed that the lower activation barrier of O 2 and the higher adsorption for CO and toluene triggered the efficient CO and toluene degradation over Pt/C 3 N 4 . Interestingly, the introduction of H 2 O (10.0 vol%) suppressed the catalytic performance of Pd/C 3 N 4 , while expedited CO and toluene oxidation over Pt/C 3 N 4 , which was revealed by DFT calculations. Furthermore, the difference in degradation intermediates, corresponding distributions and toxicity generated during toluene oxidation under different conditions over Pd/C 3 N 4 and Pt/C 3 N 4 were exposed. Compared with Pd/C 3 N 4 , less variety, toxicity and content of intermediates produced over Pt/C 3 N 4 . This work would inspire many rational designs of supported noble metal catalysts for environmentally friendly catalysis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Siyuan Hu,Mingzhen Huang,Jingru Li,Jinxin He,Kaiji Xu,Xiaoping Rao,Dongren Cai,Guowu Zhan
Herein, atomic layer deposition (ALD)-Al 2 O 3 films were applied as a medium to modulate the electronic states of the supported Pt. Based on the sacrificial template of ZIF-67, the ternary Co 3 O 4 /Pt/Al 2 O 3 catalyst exhibited better performance in catalytic CO oxidation than the binary Co 3 O 4 /Pt catalyst. Both experimental and calculation results indicate the existence of charge transport between the Pt and the ALD-Al 2 O 3 films, leading to electron-rich Pt, enhanced O 2 affinity, and reduced activation energy. Interestingly, the oxidation resistance of Pt nanoparticles was visualized when annealing Co 3 O 4 /Pt/Al 2 O 3 catalyst at high temperatures. Mechanism studies indicate the typical LH mechanism occurred in CO oxidation , showing that the co-adsorbed CO and O 2 could be converted to carbonate-type *OCOO intermediates via low energy barriers. At low temperatures, CO 2 was mainly produced by the lattice oxygen-mediated M-vK mechanism based on isotope labeling experiments. Our findings provide an alternative way to regulate the electronic states of noble metals by the ALD technique.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Manting Zhang,Tingting Zhou,Danil Bukhvalov,Fengyan Han,Caiqin Wang,Xiaofei Yang
Tri-functional PtCo/NC nanocatalysts were assembled via in-situ integration with ultralow Pt loading supported on ZIF-67 derived porous carbon material, and used as electrocatalysts for oxygen reduction reaction (ORR), ethanol oxidation reaction (EOR), hydrogen evolution reaction (HER). Detailedly, PtCo-3/NC with ultralow Pt loading (1 wt%) exhibits the halfwave potential of 0.877 V for ORR in acidic media and considerable current density for both ORR and EOR at 0.85 V, and low overpotential (η 10 =10 mV) for HER. The as-assembled zinc-air batteries (ZABs) based on PtCo/NC have higher power density than Pt/C based ZABs. DFT calculation reveals the strong metal-support interactions (MSI) in PtCo/NC, which leads to the change of electronic state, redistribution of charge density and optimization of free energy , allowing it to present greater performances than Pt/C. This work highlights the possibility of using it as highly effective electrode catalysts with ultralow Pt loading in fuel cells and metal-air battery.
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APPLIED SURFACE SCIENCE
·
2023
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IF 6.7
Yuqi Zhang,Jiasi Yan,Rixin You,Meng He,Ligen Wang,Minghui Liang
The catalytic epichlorohydrin (ECH) hydrogenation to chloro-propanol is of great industrial importance due to the extensive application of chloro-propanol as an intermediate for pharmaceutics, fine chemicals, and polymers. The challenge of this catalytic reaction lies in that dechlorination can hardly be inhibited in the selective hydrogenation of the epoxy group because the bond energy of the C-Cl bond is very close to that of the C O bond. Herein, we demonstrated that the selectivity of chloro-propanol could be improved from 82.2 % to 94.6 % by incorporating a small amount of Cu single atoms into Pt/C catalysts to inhibit dechlorination. More interestingly, the ring-opening site of the epoxy group can be also engineered by the incorporation of Cu single atoms, as evidenced by the significant increase in the selectivity of 3-chloro-1-propanol from 0.2 % to 14.5 %. Comprehensive characterizations and density functional theory (DFT) calculations were carried out to understand the interplay of Cu single atoms and Pt nanoparticles as well as its effect on the catalytic performance. The insights gained in this study will benefit the development of catalysts, especially the bimetallic catalysts for the selective hydrogenation of halogeno-aliphatic compounds.
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FUEL
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2023
·
IF 7.4
Yu Chen,Lei Jiang,Bing Bao,Chunqiang Lu,Yunkun Zhao,Shiying Chang,Dongxia Yang,Depeng Zhao,Xianming Cheng,Hua Wang,Kongzhai Li
With the improvement of current global vehicle emission standards increase and widespread application of natural gas vehicles (CNG), existing three-way catalytic converters (TWCs) need to be modified to meet the new emission regulations. In recent years, the price of palladium has been rising, while platinum, which is also used in catalytic systems, is relatively cheap, and the industry has come up with the idea of replacing palladium with platinum. Palladium loaded with a mass fraction of 1% on Ce 0.4 Zr 0.5 La 0.05 Y 0.05 O 1.95 (CZLY) did show excellent catalytic activity, however, when palladium is replaced by platinum, the catalytic activity of the catalyst for methane combustion is significantly reduced. At 680 °C under oxygen-rich conditions (20%), methane conversion can typically reach 90%. The reduced 1% Pt/CZLY catalyst, on the other hand, was unstable in activity at high temperatures, although it was significantly higher at the starting temperature (T 50 = 378 °C). In this work, it was found that the addition of niobium to CZLY improved the activity of Pt-based catalysts. The 1% Pt/Ce 0.4 Zr 0.5 La 0.05 Nb 0.05 O 2 (1% Pt/CZLN) catalysts showed a decrease in T 90 (CO) of 26 °C and T 90 (CH 4 ) of approximately 250 °C. The activity of this catalyst is consistent with that of the reduction pre-treatment 1% Pt/CZLY catalyst. Results from thermal deactivation and sulphur poisoning experiments show that the 1% Pt/CZLN catalyst exhibits superior thermal stability and anti-sulphur toxicity. For example, methane conversion of the 1% Pt/CZLN catalyst maintained at 85% at 600 °C for 32 h with a 5% decrease in activity. To clearly explain the effect of niobium doping on the catalyst, BET, XRD, H 2 -TPR, XPS and TEM tests were performed on the catalysts confirming that the strong Pt-Nb interaction stabilizes the valence state of the platinum and loads the platinum on the carrier surface in the active metallic platinum state. The amount of niobium doping was positively correlated with the metallic Pt content in the catalyst. In conclusion, the addition of niobium to platinum-based catalysts increases the methane combustion activity of the catalyst and delays thermal deactivation and sulphur poisoning of the platinum-based catalyst, extending the service life of the platinum-based catalyst.
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Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 8
·4319-4333
·
IF 11.9
Chaojie Lyu,Jiarun Cheng,Yuquan Yang,Jiwen Wu,Kaili Wu,Yunguo Yang,Woon-Ming Lau,Ning Wang,Dawei Pang,Jinlong Zheng
Highly dispersed Pt NPs anchored in hierarchically N,F co-doped hollow carbon spheres (Pt@N,F-HCS) were synthesized through a template-assisted strategy followed by fluorination and wet chemical reduction. Due to the introduction of F heteroatoms into the carbon skeleton, the degree of d–π electron conjugation between Pt NPs and N,F-HCS can be enhanced. This will lead to higher Ptx+ content in Pt species, which is beneficial for the effective adsorption of *OOH intermediates and is conducive to O–O bond breaking and triggers the direct 4-electron transfer mechanism for the ORR. In particular, the onset potential and half-wave potential values for the ORR are more positive than Pt@N-HCS without F doping, even outperforming 20%Pt/C. Besides, the Pt@N,F-HCS catalyst also possesses the smallest onset potential and largest methanol oxidation current for the MOR. In alkaline media, abundant OH− will be adsorbed around the Ptx+ sites due to its higher positive valence, and the reaction intermediate COads generated in Ptx+ sites will be further oxidized to the final product, CO2, thus improving the MOR activity and CO tolerance capacity. This heteroatom-doping strategy is favorable for enhancing the interaction between Pt NPs and the carbon-based support, and also provides insight to promote the activity and selectivity for direct methanol fuel cells.
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FUEL
·
2022
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IF 8.035
Zhuwei Yang,Xiang Gong,Linsen Li,Zhao Jiang,Riguang Zhang,Tao Fang
Liquid organic hydrogen carriers (LOHC) are considered as the promising candidates for large-scale hydrogen storage. The N -ethylcarbazole/dodecahydro- N -ethylcarbazole (NECZ/12H-NECZ) system has received increasing attention due to its excellent comprehensive properties in the hydrogen storage candidates. In this work, the Pt/SiO 2 -TiO(OH) 2 catalysts are synthesized and show good activity, selectivity and stability for 12H-NECZ dehydrogenation reaction. Among them, the 2.5 wt% Pt/SiO 2 -TiO(OH) 2 catalyst shows the best dehydrogenation performance with 5.75 wt% H 2 release amount and 98 % selectivity of NECZ. Combined with XRD, HRTEM, ATR-FTIR, XPS and EPR analysis, it is found that the oxygen vacancy concentration in Pt/SiO 2 -TiO(OH) 2 is significantly enhanced due to the formation of Si-O-Ti species compared with Pt/SiO 2 and Pt/TiO(OH) 2 , which strengthens the SMSI (strong metal-supporting interaction) effect between metal Pt and support SiO 2 -TiO(OH) 2 . The optimized d-band center of catalyst is beneficial for accelerating the sluggish kinetics of the rate-limiting step of the whole dehydrogenation reaction. Furthermore, compared with the results by replacing SiO 2 with Al 2 O 3 or CeO 2 , it is indicated that the introduction of oxides mainly plays the role of regulating the surface electronic state of TiO(OH) 2 and increasing the oxygen vacancy concentration.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Qin Wu,Ruichen Chen,Pengju Su,Daxin Shi,Yaoyuan Zhang,Kangcheng Chen,Hansheng Li
Carbon-based materials derived from metal-organic framework compounds have tunable chemical composition , morphology, and electrochemically active surface combined with good electrical conductivity and stability. In this work, Fe(OH) 3 grows on a zeolitic imidazolate framework , 2-Methylimidazole cobalt salt (ZIF-67), through oxidation and deposition. The Co 9 S 8 /NC@FeCoS 2 /NC composites with hollow yolk shell structure (HYS-Co 9 S 8 /NC@FeCoS 2 /NC) is prepared through solvothermal sulfidation combined with high-temperature carbonization using ZIF-67@Fe(OH) 3 as the precursor. A dye-sensitized solar cell assembled with HYS-Co 9 S 8 /NC@FeCoS 2 /NC as a counter electrode achieves a photovoltaic conversion efficiency of 7.07% (PCE Pt = 7.36%). The reason for this phenomenon is that the hollow yolk shell structure of Co 9 S 8 /NC@FeCoS 2 /NC material has a high specific surface area, which affords a good deal of active sites and promotes the contact between electrolyte and catalytic sites. The Fe-Co bimetal center synergies with each other to catalyze the reduction of iodide ion, showing a high catalytic activity. Besides, the material has good electrochemical stability in iodide-based electrolysis.
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