CHINESE JOURNAL OF CATALYSIS
·
2024
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IF 15.7
Zhounan Yu,Leilei Zhang,Yuanlong Tan,Rizheng Jing,Hongchen Cao,Caiyi Lou,Rile Ge,Junhu Wang,Aiqin Wang,Tao Zhang
Rh-P complexes have been widely used as catalysts for hydroformylation reactions. The extremely high price of Rh and its scarce reserves have prompted the exploration of the alternatives. In this study, we reported that Pt/PS-PPh 2 single-atom catalysts promoted by SnCl 2 were highly efficient and selective for the hydroformylation of higher α-alkenes. A broad scope of substrates (i.e., C 6 –C 12 ) were smoothly converted to the corresponding linear aldehydes with high yields under reaction conditions of 90–120 °C and 4–6 MPa syngas . The turnover frequency (TOF) was comparable to homogeneous Pt-Sn catalysts, and the linear/branched ratio reached as high as > 20. In addition, the catalyst could be reused with the extra addition of SnCl 2 . The promotional role of SnCl 2 was elucidated by quasi- in situ X-ray adsorption fine structure, Fourier transform infrared, and Mössbauer spectroscopy . It was discovered that SnCl 2 was transformed into Sn(dioxane)Cl 3 − species coordinated to Pt as a moderately electron-donating ligand, which, together with the phosphine group, stabilized mononuclear Pt (I) species against reduction and aggregation.
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RSC Advances
·
2024
·Vol. 14
·期 37
·27310-27322
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IF 3.9
Zhengjian Hou,Ke Wu,Huijie Wei,Hua Chi,Yanyan Xi,Lishuang Ma,Xufeng Lin
In this study, two series of samples (rT-Pt/TiO2 prepared with a hydrogen pretreatment and Tr-Pt/TiO2 prepared with an oxygen pretreatment) were prepared by treating commercial TiO2 supports in different atmospheres to establish different TiO2 interfacial structures, followed by the addition of platinum nanoparticles (NPs) for the catalyzed hydrogenation/dehydrogenation cycle of N-ethylcarbazole (NEC). The kinetic analysis and reaction mechanism were investigated by combining XRD, Raman, CO-DRIFT, HRTEM, XPS, H2-TPD and DFT calculations. It was found that the performance of the samples for the NEC system's cyclic hydrogen storage could be modulated by treating the TiO2 interfacial structure with different atmospheres varying the extent of strong metal-support interaction (SMSI). In addition, a turnover frequency (TOF) of 191.52 min−1 for dehydrogenation was achieved at 170 °C, which is better than the previously reported catalysts. Experimental studies (characterization and kinetic studies) and DFT calculations confirmed that the SMSI of the Tr-Pt/TiO2 series samples promoted the escape of H2 and enhanced the catalytic activity for 4H-NEC in the 12H-NEC dehydrogenation reaction. In the NEC hydrogenation reaction, the rT-Pt/TiO2 series samples were pretreated with H2 before loading platinum metal, which led to the early activation of Ti4+ in their carriers, and thus suppressed the SMSI effect of the reduction process after loading platinum. This process caused the interface formed by rT-Pt/TiO2 to have a higher energy barrier to 6H-NEC, which is an intermediate product of the NEC hydrogenation process, and this interrupted the hydrogenation process of 6H-NEC.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Xinyu Liu,Chengxiong Wang,Feng Feng,Yinglong Wu,Shiying Chang,Guangxin Liu,Dong Tian,Weinan Yang,Xianming Cheng,Dongxia Yang,Kongzhai Li,Yunkun Zhao
Catalyst deactivation caused by SO 2 poisoning generally hinders commercial viability of CO oxidation catalysts in the field of industrial flue gas purification. XPS results, CO-DRIFTS spectra and DFT calculations suggested that Pt was highly-dispersed and remained the oxidative states on SnO 2 support, resulting in that the rate-determining step of CO oxidation is to clean up the adsorbed CO and PtS 2 species is readily formed in a SO 2 -contained hydrothermal environment. It predominantly maintained metallic Pt 0 in the Pt/WO 3 catalyst, thereby led to cleaning up the activated oxygen atoms as the rate-determining step. It is very difficult to remove the sulfur species in SO 2 -poisoned catalysts within 600 °C and the mechanisms of CO oxidation are not affected by SO 2 poisoning for Pt/SnO 2 and Pt/WO 3 catalysts. These findings provide some significant insights to understand the mechanisms of CO oxidation and SO 2 -tolerance.
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TALANTA
·
2024
·
IF 5.6
Yiquan Liao,Yichang He,Bin Zhang,Ye Ma,Minggang Zhao,Ruiqi Xu,Hongzhi Cui
Glutathione (GSH) is an essential antioxidant in the human body, but its detection is difficult due to the interference of complex components in serum. Herein, hollow double-layer Pt@CeO 2 nanospheres were developed as oxidase mimetics, and the light-assisted oxidase mimetics effects were found. The oxidase activity was enhanced significantly by utilizing the synergistic effect of Schottky junction and the localized surface plasmon resonance (LSPR) of Pt under UV light . A novel GSH colorimetric-fluorescent-SERS sensing platform was established, with the sensing performance notably boosted by using the light-assisted oxidase mimetics effects. This platform boasts an exceptionally low detection limit (LOD) of 0.084 μM, while the detection time was shortened from 10 min to just 2 min. The anti-interference detection with high recovery rate (96.84%–107.4 %) in real serum made it be promising for practical application.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yuzhe Liu,Xulei Sui,Lixiao Shen,Xingshuai Lv,Longji Yuan,Anyu Li,Xueda Du,Bin Wu,Wenliang Feng,Zhen Zhang,Hong Chen,He Qi,Hui Pan,Zhenbo Wang
The popularization of proton exchange membrane fuel cells is hindered by low activity, poor stability and low utilization rate of Pt catalyst. Herein, an organic molecule layer (OML) is first in-situ directionally assembled on Pt surface via hydrogen bonding and Pt-N coordination. The amino group in OML bond with adsorbed O₂ to facilitate O–O cleavage based on hydrogen bond effect, enabling dual-channel electron acceptance and boosting the intrinsic activity of Pt by 5.5-fold. The OML also acts as a protective matrix to enhance the stability of Pt. In H₂/Air fuel cells, the catalyst achieves 1.11 W cm⁻² at 0.67 V with low Pt loading of 0.125 mg cm⁻². Notably, it delivers no current decay at 0.8 V, 10 mV potential decay at 0.8 A cm⁻², and a mere 6 % mass activity loss after 30,000 cycles. These results outperform DOE 2025 targets and state-of-the-art Pt catalysts. The OML construction strategy offers innovative concepts for high-performance Pt catalyst design and enables large-scale production.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Danfeng Xiao,Huihui Li,Hengtao Fu,Xiaofei Chen,Zelong Li,Yuhua Wang
Developing acid-tolerant photocatalysts for efficient water oxidation in unmodified Fe3+ redox media is pivotal for realizing solar energy storage via the “hydrogen farm” strategy, yet remains challenging due to intrinsic charge recombination and corrosion issues. Here, we introduce a nitrogen-doped hexagonal/tetragonal BaTa2O6 heterophase photocatalyst decorated with spatially separated Pt and CoOx cocatalysts for stable oxygen evolution in acidic Fe(NO3)3 solutions (pH 1.8). The heterophase junction, corroborated by high-resolution transmission electron microscopy (HRTEM), creates a directional built-in electric field (evidenced by surface photovoltage spectroscopy) that minimizes interfacial energy loss (<0.2 eV, confirmed by density functional theory calculations). Selective photodeposition of Pt at particle termini and CoOx on lateral surfaces spatially decouples Fe3+ reduction and water oxidation half-reactions, effectively suppressing charge recombination. Enabled by nitrogen doping-induced bandgap narrowing (light absorption up to 630 nm), the optimized catalyst achieves an unprecedented O2 evolution rate of 124 μmol h−1 under visible light, with apparent quantum efficiencies of 10.5% at 420 nm and 0.3% at 600 nm. The system maintains over 93% activity for 12 h and demonstrates robust compatibility with Fe2+/Fe3+ redox cycling, confirmed by the stoichiometric production of H2/O2 (2 : 1) in a Z-scheme overall water splitting configuration. This work establishes a novel heterophase engineering approach for designing acid-stable photocatalysts, offering a promising pathway toward practical solar-to-chemical energy conversion.
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BIOELECTROCHEMISTRY
·
2026
·
IF 4.9
Zijie Pi,Yuanyuan Zhang,Rongqin Yang,Lin Liu,Yu Huang,Yingchi Wu,Tao Gou,Honghao Kang,Tao Zhang,Xiaoling Yang,Xiaoling Liao
A high-performance nanozyme electrochemical sensor was engineered for the sensitive detection of hydrogen peroxide (H 2 O 2 ). The sensor is based on a synergistic ternary nanocomposite of ZIF-8, reduced graphene oxide (RGO), and platinum nanoparticles (Pt NPs). In this design, the Pt NPs serve as the catalytic centers with intrinsic peroxidase-like activity, effectively mimicking natural enzymes to catalyze the electrochemical reduction of H 2 O 2 . This nanocomposite was immobilized on a glassy carbon electrode (GCE) via a combined drop-casting and electrodeposition strategy. Morphological and structural analyses using scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), and X-ray photoelectron spectroscopy (XPS) confirmed the successful fabrication of a uniform nanocomposite architecture. Systematic optimization revealed that the sensor exhibited excellent detection performance for H 2 O 2 , with a sensitivity of 22.3 μA mM −1 cm −2 ( n = 4), a detection limit as low as 59 nM (S/N = 3), a limit of quantification of 0.197 μM, and a linear range of 62 nM–13.07 mM, exhibiting good selectivity and reproducibility. Importantly, the sensor was successfully applied for the real-time, in-situ monitoring of H 2 O 2 released from zebrafish embryos under cadmium ion (Cd 2+ ) induced oxidative stress. This work offers a promising tool for the early assessment of heavy metal-induced oxidative damage.
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MICROCHEMICAL JOURNAL
·
2025
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IF 5.1
Guoni Huang,Jiezhen Pan,Junfang Zhu,Ye Zhang,Xiaohe Zhang,Shihua Luo
In this study, we introduce an ultrasensitive electrochemical RNA biosensor based on hyperbranched primer exchange reaction (HPER) cascade amplification and Au@Pt@UiO-66-NH 2 nanozymes. This strategy employs catalytic hairpin assembly (CHA) for precise target RNA recognition, which trigger the immobilization of HPER products onto the electrode surface, thereby providing binding sites for nanozymes. Then, the sDNA@Au@Pt@UiO-66-NH 2 signal probes (sDAPU probes) attach to the HPER scaffolds through base-pairing interactions, facilitating signal amplification. The nanozymes catalyze the decomposition of hydrogen peroxide into H 2 O and O 2 , producing a significantly amplified electrochemical signal. By combining CHA-HPER cascade amplification with the catalytic activity of sDAPU probes, the established biosensor achieves remarkable sensitivity, with a detection limit as low as 14.68 aM, and high specificity that enables the differentiation of non-target pathogen RNA. Furthermore, the biosensor also demonstrates excellent recovery rates in serum samples. Therefore, this electrochemical strategy shows great potential as a diagnostic tool for ultrasensitive Mycobacterium tuberculosis detection.
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ACS Applied Materials & Interfaces
·
2013
·
IF 5.008
Xiong Yin,Fan Wu,Nianqing Fu,Jing Han,Dongliang Chen,Peng Xu,Meng He,Yuan Lin
A high-performance Pt-free counter electrode (CE) based on poly(3,4-ethylenedioxythiophene) (PEDOT) film for plastic dye-sensitized solar cells (DSCs) has been developed via a facile solid-state polymerization (SSP) approach. The polymerization was simply initiated by sintering the monomer, 2,5-dibromo-3,4-ethylenedioxythiophene (DBEDOT), at the temperature of 80 °C, which can be applied on the plastic substrate. The cyclic voltammetry measurements revealed that the catalytic activity of the SSP-PEDOT CE for triiodide reduction is comparable with that of the Pt CE. Under optimized conditions, the power conversion efficiency of a DSC with a N719-sensitized TiO2 photoanode and the SSP-PEDOT CE is 7.04% measured under standard 1 sun illumination (100 mW cm–2, AM 1.5), which is very close to that of the device fabricated under the same conditions with a conventional thermally deposited Pt CE (7.35%). Furthermore, taking advantage of the compatibility of the SSP-PEDOT with the plastic substrates, a full plastic N719-sensitized TiO2 solar cell was demonstrated, and an efficiency of 4.65% was achieved, which is comparable with the performance of a plastic DSC with a sputter-deposited Pt CE (5.38%). These results demonstrated that solid-state polymerization initiated at low temperature is a facile and low-cost method of fabricating the high-performance Pt-free CEs for plastic DSCs.
研究领域:
材料科学
·
光伏技术
·
高分子化学
·
能源材料
·
薄膜技术
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BIOSENSORS & BIOELECTRONICS
·
2023
·
IF 12.6
Limin Yang,Heng Guo,Ting Hou,Jingang Zhang,Feng Li
Breast cancer (BC) is the most common cancer in the world and circulating tumor cells (CTCs) are reliable biomarkers for early breast cancer diagnosis in a non-invasive manner. However, effective isolation and sensitive detection of BC-CTCs by portable devices in human blood samples are extremely challenging. Herein, we proposed a highly sensitive and portable photothermal cytosensor for direct capture and quantification of BC-CTCs. To achieve efficient isolation of BC-CTCs, aptamer functionalized Fe 3 O 4 @PDA nanoprobe was facilely prepared through Ca 2+ -mediated DNA adsorption. To further detect the captured BC-CTCs with high sensitivity, multifunctional two-dimensional Ti 3 C 2 @ [email protected] nanozyme was synthesized, which not only possessed superior photothermal effect but also exhibited high peroxidase-like activity for catalyzing 3,3′,5,5′-tetramethylbenzidine (TMB) to produce TMB oxide (oxTMB) with a strong photothermal characteristic, combining with Ti 3 C 2 @ [email protected] to synergistically amplify the temperature signal. Moreover, numerous Ti 3 C 2 @ [email protected] nanocomposites would be selectively attained on the BC-CTCs surface through multi-aptamer recognition and binding strategy, which further enhanced the specificity and facilitated signal amplification . Therefore, direct separation and highly sensitive detection of BC-CTCs was successfully achieved in human blood samples. More significantly, the controlled release of the captured BC-CTCs without affecting cell viability could be straightforwardly realized by a simple strand displacement reaction. Thus, with the distinct features of portability, high sensitivity, and easy operation, the current method holds great promise for early diagnosis of breast cancer.
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FUEL
·
2022
·
IF 8.035
Ruolan Li,Zongqian Wu,Ya Chen,Xingyan Liu,Weiwei Guo,Yumin Huang,Min Fu,Youzhou He
An efficient bifunctional porphyrin-based MOF is fabricated for photocatalytic hydrogen evolution and NO removal, in which the mixed Zr/Ti-oxo clusters are the metal nodes and uniformly distributed Pt nanoparticles (Pt NPs) are the co-catalysts. It is worth noting that the optimal Zr-MOF-s(Pt)(Zr/Ti)-R is obtained through replacing partial Zr(IV) with Ti(IV) in the original Zr-based porphyrin MOFs and in-situ generating confined Pt NPs with a relatively small size within the internal cavities. Compared with the majority of reported Zr-based porphyrin MOFs, the Zr-MOF-s(Pt)(Zr/Ti)-R exhibits an extremely high hydrogen evolution activity (2545.11 μmol·g −1 ·h −1 ) and NO removal rate (46.6 %) under visible light irradiation. The excellent photocatalytic performance should be ascribed to the reason that the mixed Zr/Ti-oxo cluster and the in-situ generated Pt NPs significantly promote the rate of charge transfer and separation. Moreover, the photocatalytic NO oxidation process was also monitored by in - situ DRIFTS, which indicates the Zr-MOF-s(Pt)(Zr/Ti)-R could realize the effective oxidation of NO and intermediates to the final product (NO 3 – ). This work provides us with a practical route to further improve the photocatalytic performance by synergistically modifying the original metal clusters to adjust the ligand-to-metal charge transfer efficiency and in-situ introducing metal nanoparticles to form Schottky junctions.
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JOURNAL OF MEDICINAL CHEMISTRY
·
2023
·
IF 7.3
Xiao-Meng Liu,Zhe Li,Xin-Ru Xie,Jia-Qian Wang,Xin Qiao,Xin Qiao,Cheng-Zhi Xie,Jing-Yuan Xu
Exploring multi-targeting chemotherapeutants with advantages over single-targeting agents and drug combinations is of great significance in drug discovery. Herein, we employed phytogenic evodiamine (EVO) and conventional Pt(II) drugs to design and synthesize multi-target EVO–Pt(IV) anticancer prodrugs (4–14). Among them, compound 10 exhibited a 118-fold enhancement in the IC50 value compared to cisplatin and low toxicity to normal cells. Further studies proved that 10 significantly enhanced intracellular Pt accumulation and DNA damage, perturbed mitochondrial membrane potential, inhibited cell migration and invasion, upregulated reactive oxygen species levels, and induced apoptosis and autophagic cell death. Molecular docking assay revealed that 10 fits perfectly into the extracellular signal-regulated protein kinase (ERK)-1 pocket, which was verified to produce profound ERK suppression. Most strikingly, compound 10 exhibited superior in vivo antitumor efficiency and effectively attenuated systemic toxicity. Our results emphasize that functionalizing platinum drugs with the multi-target EVO could generate synergistically excellent anticancer activity with low toxicity and decreased resistance, which may represent a brand-new cancer therapy modality.
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