ELECTROCHIMICA ACTA
·
2015
·
IF 4.504
Guiqiang Wang,Shuai Kuang,Juan Zhang,Shuo Hou,Siming Nian
A graphitic carbon nitride (g-C 3 N 4 )/multiwalled carbon nanotubes (MWCNT) composite is prepared by a combination of refluxing process and heating polymerization and investigated as the counter electrode in dye-sensitized solar cells. SEM and TEM studies indicate that MWCNT is very well incorporated and attached to g-C 3 N 4 . Electrochemical impedance spectroscopy demonstrates that the charge-transfer resistance of g-C 3 N 4 /MWCNT composite electrode is 2.1 Ω cm 2 , which is much lower than those of the individual g-C 3 N 4 and MWCNT electrodes. This enhanced electrocatalytic activity is beneficial for improving the photovoltaic performance of dye-sensitized solar cells. Under illumination of 100 mW cm −2 , the dye-sensitized solar cell based on g-C 3 N 4 /MWCNT counter electrode achieves a conversion efficiency of 6.34%, which is comparable to that of the cell based on Pt counter electrode.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 35
·13967-13978
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IF 3.069
Qiang Ning,Huaike Zhang,Yurong He,Zhiqiang Chen,Suyao Liu,Jie Ren
Small Pt particles (about 1.2 nm) were highly dispersed on ZSM-22 zeolites via a strong electrostatic adsorption (SEA) method and exhibited a promotion effect on the catalytic performance in n-dodecane isomerization in comparison with the conventional catalyst. Several promoters (Ce, La, and Re) were introduced to further improve the aggregation resistance of the small Pt particles. A series of characterization including H2-TPR, XPS and STEM as well as DFT calculations provided solid evidence that the strong interaction between Pt and promoter species not only effectively hinders the Pt aggregation but also alters the electronic state of the Pt sites. Moreover, Ce and La promoters also lead to a slightly improved amount of B acid sites determined by Py-FTIR. Thus, improved activity and selectivity were achieved on a Ce-modified catalyst due to the better balanced bifunctionality between the slightly increased acidity of zeolites and electron-deficiency of Pt. The electron-rich Pt sites are responsible for the significant increase of CH4 selectivity and the decrease of total isomer selectivity in n-dodecane isomerization. In addition, a high-temperature reduction test revealed the higher isomerization activity and selectivity (about 10% higher than the unmodified catalyst) of the Ce-modified catalyst owing to the strong bond of Pt–O–Ce, further confirming the positive effect of the Ce promoter on the sintering resistance of small Pt particles.
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RSC Advances
·
2016
·Vol. 6
·期 74
·70303-70310
·
IF 3.289
Hongxing Zhang,Yiwei Zhang,Yuming Zhou,Chao Zhang,Xiaoli Sheng,Shuo Zhao,Jiasheng Fang,Mingyu Zhang
This article reports a facile and controllable one-step method to construct Pt@hollow mesoporous SiO2 (Pt@HMSiO2) nanoparticles (NPs). To enhance the catalytic activity, cerium species were impregnated into Pt@HMSiO2 NPs, fabricating highly reactive Pt–CeO2@HMSiO2 NPs. To verify the successful synthesis of the Pt@HMSiO2 and Pt–CeO2@HMSiO2 NPs, and study the influence of CeO2 species on the catalytic performance, the as-prepared NPs were characterized by several techniques, including SEM, TEM, EDX, FTIR, XRD, BET and UV-vis analyses. In this work, the reduction of 4-NP was employed as a model reaction to test the catalytic performance. Compared to Pt@HMSiO2, the Pt–CeO2@HMSiO2 NPs show higher catalytic activity, because of the co-catalysis of CeO2 NPs. However, the excess amount of CeO2 NPs would lead to a lower catalytic activity, due to the blocking of the catalyst pore. In addition, the Pt–CeO2@HMSiO2 NPs show a high thermal stability due to the protection of the SiO2 shell. Meanwhile, we have also used the reaction of propane dehydrogenation to further verify the excellent catalytic stability of Pt–CeO2@HMSiO2 NPs. This strategy is novel, albeit efficient, and can be extended to the preparation of other nanocatalysts.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Aicaijun Zhang,Pengyu Dong,Yan Wang,Kangjie Gao,Jinkang Pan,Bairen Yang,Xinguo Xi,Jinlong Zhang
It is still challenging to fabricate photocatalysts via loaded metal cocatalysts with good dispersion onto the conjugated polymers (CPs). Herein, a donor-acceptor (D–A) structural CP of PyDTDO-3 was employed to host platinum (Pt) nanoparticles (NPs) using N , N ′-dimethylformamide (DMF) as a protectant, stabilizer, and reducing agent, which not only promotes Pt NPs to have excellent dispersion property on the surface of PyDTDO-3 but also endows Pt NPs to maintain metallic Pt 0 species. As a result, the PyDTDO-3 loaded with Pt NPs exhibits remarkable hydrogen (H 2 ) evolution activity with a rate of 39.9 mmol g −1 h −1 under visible light irradiation, and the fair stability of optimal 7% Pt/PyDTDO-3 is expressed in the rate of H 2 generation upon 30 h cycling. Based on density functional theory (DFT) calculations, it has been demonstrated that Pt NPs are selectively loaded onto the acceptor (A) unit of PyDTDO-3 that has the lowest adsorption energies ( E ads ) and the closest bond lengths between the Pt NPs and PyDTDO-3. Moreover, there are much more electrons filling at the Fermi level ( E f ), indicating the optimal 7% Pt/PyDTDO-3 with high electroconductivity timely captured and removed the photoinduced electrons and thus realized the space separation efficiency of electron-hole pairs. Overall, our findings offer a rational way to load metal cocatalysts onto CPs with good dispersion for efficient photocatalytic H 2 evolution.
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BIOSENSORS & BIOELECTRONICS
·
2017
·
IF 7.78
Yujie Yu,Chao Yu,Yazhen Niu,Jun Chen,Yilin Zhao,Yuchan Zhang,Rufei Gao,Junlin He
We designed an amplified detection strategy for the sensitive determination of lead ions (Pb 2+ ) based on a target-triggered nuclear acid cleavage of Pb 2+ -specific DNAzyme as a selectivity interface combined with Pd-Pt alloys modified Fe-MOFs (Fe-MOFs/PdPt NPs) hybrids acting as the signal tag. Streptavidin modified reduced graphene oxide-tetraethylene pentamine-gold nanoparticles (rGO-TEPA-Au) served as a sensor platform for immobilizing more DNAzyme. In the presence of Pb 2+ , the substrate DNA strand can be specifically cleaved at the ribonucleotide site by DNAzyme to produce a new single-DNA on the interface. Then, the hairpin DNA with hybrid strand matched by its complement to the single-DNA was employed to modify the Fe-MOFs/PdPt NPs bioconjugates for signal amplification . Fe-MOFs/PdPt NPs catalyze hydrogen peroxide (H 2 O 2 ) to produce the electrochemical signal which was recorded by chronoamperometry . Benefiting from the Pb 2+ -dependent DNAzyme, the proposed method can selectively detect Pb 2+ in the presence of other metal ions . The newly designed biosensor exhibited a good linear relationship ranging from 0.005 to 1000 nmol L −1 with a low detection limit of 2 pM (S/N = 3) for Pb 2+ . This Pb 2+ -dependent DNAzyme based ultrasensitive biosensor showed high sensitivity and selectivity, providing potential application for Pb 2+ detection in naturally contaminated sewage and spiked drinking water samples.
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FUEL PROCESSING TECHNOLOGY
·
2025
·
IF 7.7
Yi Lin,Yulong Wang,Hongxiang Huang,Feng Wang,Zaixing Wang,Shi Jiang,Xiaoqin Liu,Yu Guo
This study focuses on a Pt-promoted Ni/NiAl (Ni/NiO-Al 2 O 3 ) catalyst for butane steam reforming, designed to overcome hydrothermal oxidation and sulfur poisoning in Ni-based systems. A series of Ni/Al (Ni/Al 2 O 3 ) and Ni/NiO-Al 2 O 3 catalysts, with and without Pt modification, were synthesized and systematically evaluated under severe reforming conditions. Compared with conventional Ni/Al, Ni/NiAl exhibited stronger metal-support interaction through NiAl 2 O 4 formation but suffered rapid deactivation in steam-rich and sulfur-containing atmospheres. Incorporating 0.5 wt% Pt markedly improved stability, maintaining high activity and hydrogen selectivity during both steam and H 2 S exposure. Characterization by XRD, TEM, H 2 -TPR, and XPS revealed that Pt induces a synergistic protection mechanism, in which hydrogen spillover dynamically regenerates oxidized Ni species and weakens Ni S interactions. This effect reduces sulfur coverage on active Ni sites, preserving highly dispersed metallic Ni 0 . Time-resolved outlet gas analysis further indicated that sulfur preferentially deactivates reforming sites, followed by progressive inhibition of the water-gas shift reaction via a COS-mediated pathway. The catalyst demonstrated excellent stability under 5 ppm H 2 S at 850 °C, confirming the dual protective role of Pt against oxidation and sulfur poisoning. These findings provide mechanistic insights and design principles for robust, regenerable Ni-based catalysts tailored for distributed hydrogen production from LPG.
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高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Zhenyu Wei,Jian-Qiu Huang,Qing-An Huang
Variations in surface-adsorbed mass linearly shift the frequency of piezoelectric sensors, thereby enabling precise measurement of target molecules and facilitating applications in biological and gas sensing. The growing demand for high-precision piezoelectric sensors has spurred research into enhancing sensitivity, including the optimization of sensing materials and resonant modes. This study introduces an approach to enhancing the sensitivity of piezoelectric sensors by utilizing the Exceptional Point (EP) in Parity-Time (PT)-symmetric systems. By capacitively coupling an external LC circuit with a nonlinear negative resistance to the piezoelectric sensor, we transform the sensor into a PT-symmetric system with linear loss and nonlinear gain. Both theoretical and experimental results reveal that when an asymmetric perturbation is applied to the loss resonator, the eigenfrequency of the nonlinear PT-symmetric system biased at the EP exhibits a cube-root singularity. The nonlinearly saturated gain can eliminate the imaginary part of the eigenfrequency and suppress noise. A Film Bulk Acoustic Resonator (FBAR) sensor coated with a cellulose acetate (CA)/graphene oxide (GO) composite was fabricated and characterized. An experimental PT-symmetric system was constructed using the CA/GO-FBAR sensor. The humidity perturbation experiments demonstrate that the PT-symmetric FBAR sensor system achieves a significant sensitivity enhancement under small perturbations. This novel approach overcomes the traditional limitations related to materials and structures for sensitivity enhancement. Furthermore, the concept of PT symmetry could be extended to other piezoelectric sensors for biological and gas sensing, thereby enabling high-sensitivity detection of trace target molecules via the integration of diverse sensitive materials.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Ping Yu,Lin Wang,Huan Liu,Anfeng Yu,Xinmei Liu,Zhe Yang
Developing reliable and cost-effective optical hydrogen sensors detecting hydrogen leakage at room temperature is of paramount importance. It requires that hydrogen sensors show a rapid and significant color change in low concentration H 2 /air mixtures, which remains challenging. Herein, we demonstrate an eye-readable hydrogen sensor based on Pt decorated hexagonal WO 3 (W 0 /300/Pt). It is evidenced W 0 /300/Pt exhibits excellent gasochromic properties, with reflectivity differences of 78% and 73% and fast coloring times of 3.10 s and 2.64 s in 10% H₂/Ar and 10% H₂/air. Moreover, W 0 /300/Pt shows an obvious color change from light gray to dark blue finally with ΔE value of 71, and exhibits a detect limitation less than 0.1% H 2 in 1 s. The gasochromic mechanism related to crystalline phase structure was unveiled via in situ characterization techniques. This study also presents novel evidence that bolsters the “localized water molecules” model and provides theoretical insights for the advancement of highly sensitive WO 3 gasochromic materials.
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JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Hongbing Wang,Yifei Yang,Shixiang Yu,Beibei Zhang,Junzhong Xie,Jun Chen,Dongping Wang,Bomin Feng,Changyin Zhong,Linsen Zhou,Wei Cui,Ding Ma,Yunxi Yao
Liquid-phase hydrogen isotopes exchange between hydrogen and water is a promising route for the hydrogen isotopes separation from water, catalyzed by the metal Pt with hydrophobic coating to surmount the flooding of reactive sites. However, poor water activation ability on Pt has limited the catalytic efficiency of Pt-based catalysts and hindered their application. Herein, we report a bifunctional Pt/ZSM-5 catalyst with hydrophobic modification by surface silylation for H 2 -HDO isotope catalytic exchange. The integration of metallic Pt and Brønsted acid (BA) sites in the microporous ZSM-5 boosts the catalytic efficiency of deuterium extraction by two orders of magnitude compared to commercial Pt-C at the optimum condition. In-situ spectroscopic and theoretical studies demonstrated that HDO-H 2 O preferentially adsorbs on BA sites (-Si-OH-Al) to form protonated water clusters stabilized by hydrogen-bonded network or to undergo the proton exchange to leave deuterium on zeolite framework as a new acidic site ([AlO 4 D]). Under the attractive interaction, the dissociated hydrogen on Pt clusters releases partial electrons to form positively-charged hydrogen, which further transfers to the [AlO 4 D] sites or protonated water clusters by interfacial spillover to produce the overcharging intermediates. These intermediates cleave their O-D bonds to form positively charged D, which ultimately spills back to Pt cluster and combines with the remaining electron to desorb in the form of HD. The synergistic effect between Pt and BA sites creates a new pathway of hydrogen transfer, which enables the more efficient hydrogen-water isotope exchange on the bifunctional Pt/ZSM-5 catalyst.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2016
·Vol. 22
·期 29
·9909-9913
·
IF 5.771
Wenhai Wang,Jing Geng,Long Kuai,Min Li,Baoyou Geng
Graphical Low cost, high value : An Mn 2 O 3 catalyst with porous structure exhibits comparably activity to commercial Pt/C and notably higher activity than other Mn-based oxides, such as Mn 3 O 4 and MnO 2 . In light of the low cost and high earth abundance of Mn, the highly active Mn 2 O 3 is a promising candidate to be used as a cathode material in metal–air batteries and alkaline fuel cells. Preparing nonprecious metal catalysts with high activity in the oxygen reduction reaction (ORR) can promote the development of energy conversion devices. Support-free porous Mn 2 O 3 was synthesized by a facile aerosol-spray-assisted approach (ASAA) and subsequent thermal treatment, and exhibited ORR activity that is comparable to commercial Pt/C The catalyst also exhibits notably higher activity than other Mn-based oxides, such as Mn 3 O 4 and MnO 2 . The rotating ring disk electrode (RRDE) study indicates a typical 4-electron ORR pathway on Mn 2 O 3 . Furthermore, the porous Mn 2 O 3 demonstrates considerable stability and a good methanol tolerance in alkaline media. In light of the low cost and high earth abundance of Mn, the highly active Mn 2 O 3 is a promising candidate to be used as a cathode material in metal–air batteries and alkaline fuel cells.
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JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Xing Qian,Hongyu Liu,Yixuan Huang,Zejia Ren,Yating Yu,Chong Xu,Linxi Hou
Transition metal chalcogenides with yolk-shell nanostructures are a family of promising electrocatalytic materials with complex interior construction and remarkable structural tenability. In this work, a sequence of yolk-shell transition metal sulfide nanospheres (Co-Ni-MoS x , Co-MoS x and Ni-MoS x ) are prepared as superior Pt-free catalysts for dye-sensitized solar cells. This yolk-shell structure, consisting of a thin shell and an inner porous core, exposes more active sites and provides more contact regions between the electrolyte and catalyst. By comparing with the ternary Co-MoS x and Ni-MoS x nanospheres , the quaternary Co-Ni-MoS x nanospheres have advantages of the relatively larger surface area , favourable chemical composition , higher conductivity and excellent catalytic performance for expediting the reduction of I 3 − in solar cells. Particularly, as for Co-Ni-MoS x , a splendid power conversion efficiency of 9.76% is achieved under a standard irradiation, which is much better than that of Pt (8.24%).
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Hao Zhang,Qiuye Li,Bowen Li,Bo Weng,Zhihong Tian,Jianjun Yang,Johan Hofkens,Feili Lai,Tianxi Liu
We report a porous metal–organic framework loaded with single Pt atoms, namely PCN-222(Pt) nanorods, which are prepared by the self-assembly of Pt-metalized tetrakis(4-carboxyphenyl)porphyrin ligand with a Zr 6 cluster. The mass-loading of Pt in the synthesized PCN-222(Pt) is up to 4.67%, and can be accurately controlled by using an in-situ reaction strategy. Remarkably, the PCN-222(Pt) exhibits a highly efficient photocatalytic hydrogen production rate of 614 μmol g -1 h −1 , which is 7.4 times higher than that of PCN-222 (an isostructural sample to PCN-222(Pt) without coordinated Pt ions in the porphyrin rings). The apparent quantum efficiency of PCN-222(Pt) reaches up to 1.049% at 420 nm. Electron paramagnetic resonance spectra confirm the as-formed intermediate Zr III , obtained from the reduction of Zr IV species, participates in the photocatalytic reaction. Density functional theory calculations demonstrate the positive role that single Pt atoms in PCN-222(Pt) play in optimizing the corresponding hydrogen binding energy. The existence of this dual reaction mechanism in PCN-222(Pt) greatly and synergistically boosts the photocatalytic H 2 production activity.
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