CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2023
·
IF 2.2
Qian Liu,Yingyi Wen,Jian-Ze Xiao,Shao-Zhen Luo,Guan-E Wang,Peng-Yi Tang,Xiao-Liang Ye,Gang Xu
The poor sensitivity of metal-oxide (MO) sensing material at room temperature can be enhanced by the modification of noble metal catalysts . However, the large size and uncontrollable morphology of metal nanoparticles (NPs) compromise the catalytic activity and selectivity. Downsizing metal NPs to the atomic level is a promising solution because it offers high activity and selectivity. Nevertheless, a facile and universal approach for stable loading atomic-level metal on MO-based sensing materials is still challenging. Herein, we present a strategy to construct synergetic coordination interface for uniform loading of atomic-level metal catalysts on MO-based gas-sensing materials using a difunctional mediator layer. In this work, atomically dispersed Pt catalysts are coordinately anchored on ZnO nanorods (NRs) using polydopamine (PDA) as a mediator. As a result, compared with pristine ZnO NRs, a six-fold enhanced response of 18,489% is achieved toward 100 ppm NO 2 on 0.20 wt%Pt–ZnO@PDA-1.5 nm, and the selectivity is also promoted. Such sensitivity is higher than that of most reported noble metal-modified MO NO 2 -sensing materials. This work provides a simple and general strategy for building highly sensitive and selective gas-sensing materials using atomic-level noble metal catalyst.
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Materials Today Energy
·
2023
·
IF 9.3
Man Zhou,Suting Xue,Qin Feng,Xuan Liang,Wangchen Wu,Yanli Zhou,Minmin Ni,Xudong Zheng,Song Xu,Jin Zhao,Zhongyu Li
Noble metal nanoparticles (NMNPs) modified semiconductors play important roles in heterogeneous catalysis . However, for the ultra-small NMNPs (<5 nm) on TiO 2 , the problems of easy agglomeration and quick deactivation highlight the need for highly efficient protection of ultra-small NMNPs. Here, we introduce a novel structure of carbonized liquid crystals (CLCs) protected Pt NPs on TiO 2 , which involves in-situ photo-reduction of chloroplatinic acid to ultra-small Pt NPs in lamellar liquid crystals. According to the results of morphological structures, CLCs changed the contact type of Pt/TiO 2 from ‘face-contact’ to ‘point-contact’, which was consistent with our simulation results. Compared with the bare Pt/TiO 2 , the visible-light photocatalytic H 2 production rate of C–Pt/TiO 2 exhibited 1.75-fold enhancement under the protection of CLCs (26.73 mmol g −1 h −1 vs. 15.26 mmol g −1 h −1 ). Especially, the marriage of CLCs and the traditional Pt/TiO 2 photocatalyst achieved long-term stability, which remained 87% of the original rate at the sixth cycle.
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Small Methods
·
2023
·Vol. 7
·期 7
·2300121
·
IF 12.4
Gaoyan Xiong,Chao Feng,Hsiao-Chien Chen,Junxi Li,Fei Jiang,Shu Tao,Yunxia Wang,Yichuan Li,Yuan Pan
This study adopts a facile and effective in situ encapsulation-oxidation strategy for constructing a coupling catalyst composed of atomically dispersed Pt-doped Co 3 O 4 spinel nanoparticles (NPs) embedded in polyhedron frames (PFs) for robust propane total oxidation. Benefiting from the abundant oxygen vacancies and more highly valent active Co 3+ species caused by the doping of Pt atoms as well as the confinement effect, the optimized 0.2Pt-Co 3 O 4 NPs/PFs catalyst exhibits excellent propane catalytic activity with low T 90 (184 °C), superior apparent reaction rate (21.62×10 8 (mol g cat −1 s −1 )), low apparent activation energy ( E a = 17.89 kJ mol −1 ), high turnover frequency ( 811×10 7 (mol g cat −1 s −1 )) as well as good stability. In situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory calculations indicate that the doping of Pt atoms enhances the oxygen activation ability, and decreases the energy barrier required for C H bond breaking, thus improving the deep oxidation process of the intermediate species. This study opens up new ideas for constructing coupling catalysts from atomic scale with low cost to enhance the activation of oxygen molecules and the deep oxidation of linear short chain alkanes at low temperature.
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ADVANCED MATERIALS
·
2023
·Vol. 35
·期 36
·2301310
·
IF 29.4
Zichen Wang,Suhao Chen,Wei Wu,Runzhe Chen,Yu Zhu,Haoran Jiang,Liyue Yu,Niancai Cheng
The sluggish kinetics of oxygen reduction reaction (ORR) and unsatisfactory durability of Pt-based catalysts are severely hindering the commercialization of proton-exchange-membrane fuel cells (PEMFCs). In this work, the lattice compressive strain of Pt-skins imposed by Pt-based intermetallic cores is tailored for highly effective ORR through the confinement effect of the activated nitrogen-doped porous carbon (a-NPC). The modulated pores of a-NPC not only promote Pt-based intermetallics with ultrasmall size (average size of <4 nm), but also efficiently stabilizes intermetallic nanoparticles and sufficient exposure of active sites during the ORR process. The optimized catalyst (L1 2 -Pt 3 Co@ML-Pt/NPC 10 ) achieves excellent mass activity (1.72 A mg Pt −1 ) and specific activity (3.49 mA cm Pt −2 ), which are 11- and 15-fold that of commercial Pt/C, respectively. Besides, owing to the confinement effect of a-NPC and protection of Pt-skins, L1 2 -Pt 3 Co@ML-Pt/NPC 10 retains 98.1% mass activity after 30 000 cycles, and even 95% for 100 000 cycles, while Pt/C retains only 51.2% for 30 000 cycles. Rationalized by density functional theory, compared with other metals (Cr, Mn, Fe, and Zn), L1 2 -Pt 3 Co closer to the top of “volcano” induces a more suitable compressive strain and electronic structure on Pt-skin, leading to an optimal oxygen adsorption energy and a remarkable ORR performance.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Qiangqiang Wu,Hanke Li,Guangxing Yang,Yonghai Cao,Hongjuan Wang,Feng Peng,Hao Yu
A variety of adsorbed intermediates have been extensively assigned during CO 2 hydrogenation on Pt/γ-Al 2 O 3 . However, the surface sites where the surface species reside have not been well resolved, which are extremely important to depict the reaction pathways of CO 2 hydrogenation. In the current work, surface species adsorbed on three regions were distinguished by in situ diffuse-reflectance infrared Fourier transform spectroscopy, i.e., contiguous Pt region of Pt nanoparticle, interfacial Pt int -O-Al int region between Pt nanoparticle and γ-Al 2 O 3 , and surface region of γ-Al 2 O 3 away from Pt nanoparticle. The dynamics of adsorbed H species, carbonyl species, bicarbonates, formate species, and adsorbed CO 2 , were identified at different sites, proving that the reaction occurs at the Pt/γ-Al 2 O 3 interface. We found that only the C-containing species at the Pt perimeter are directly active intermediates for the reaction. Such spatial analysis bridges the gap between the hydrogen activation and CO 2 activation, providing a deep understanding of CO 2 hydrogenation. In addition, the interface structure with oxygen vacancy is important for CO 2 activation, driving the reaction through carboxylate (*HOCO) pathway to form CO at the interface rather than formate (*HCOO) pathway and then be hydrogenated at the Pt surface.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yanyan Song,Ruxangul Jamal,Tursun Abdiryim,Abdukeyum Abdurexit,Shuyue Xie,Lielie Liu,Mariyam Niyaz,Nawrzhan Serkjan,Yu Zhang
The electricity generated by direct methanol fuel cells (DMFCs) comes from methanol oxidation reaction (MOR), which is affected by electrocatalytic activity of anode materials . Herein, Pt nanoparticles supported by the composite of thiol group grafted poly(3,4-propylenedioxythiophene) (PProDOT-2CH 2 SH) and Ni–N co-doped bamboo-like carbon nanotubes (Ni-NCNT) are prepared and proposed as an anode material for DMFCs. The results from morphological analysis show that the Pt nanoparticles uniformly disperse on the surface of support (PProDOT-2CH 2 SH/Ni-NCNT) with bamboo-like structure, and there is an electronic effect between the Pt and Ni confirmed by X-ray photoelectron spectroscopy analysis. Electrochemical tests reveal that the PProDOT-2CH 2 SH/Ni-NCNT/Pt catalyst demonstrates good electrocatalytic activity for the MOR in acidic electrolyte, and the catalyst has higher resistance to CO poisoning than commercial Pt/C. The mass activity (MA) of catalyst is up to 1670.54 mA mg Pt −1 with an electrochemical active surface area (ECSA) of 98.0 m 2 g −1 , and the catalyst maintains good performance after 800 cycles. This work provides a high-performance MOR catalyst in practical application for DMFCs.
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Yujie Li,Yuanyuan Liu,Zeyan Wang,Peng Wang,Zhaoke Zheng,Hefeng Cheng,Ying Dai,Baibiao Huang
Photocatalytic H 2 O 2 evolution has received extensive attention as an environmentally friendly method, which is a dynamic process of formation and decomposition. At present, researches mainly focus on the H 2 O 2 formation, while the decomposition of H 2 O 2 is rarely studied. In addition, platinum as a cocatalyst plays an important role in enhancing the photocatalytic activity, but the effects of platinum valence state on the activity, especially towards H 2 O 2 formation and decomposition, has not been studied in detail to the best of our knowledge. In this work, platinum with different valence state were deposited onto boron containing metal organic frameworks (UiO-67-B), and the roles of Pt(0), Pt(II) and Pt(IV) in the photocatalytic H 2 O 2 process were explored in detail. Both the experimental results and theoretical calculations indicate that the presence of Pt(II) plays an important role not only in promoting the H 2 O 2 formation but also in inhibiting the H 2 O 2 decomposition.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Xiaoqing Jiang,Jie Zou,Yongjian Ni,Yuheng Wang,Xianwei Qian,Xuebin Li,Shihao Wei,Yuanjie Su,Guangzhong Xie,Mingjun Zhou,Jiawen Jian
The catalytic activity of an oxygen-pumping electrode is very important to the performance of amperometric NO x (NO and NO 2 ) sensors. To enhance the stability of electrochemical NO x sensors based on Pt electrodes, we fabricated sensitive electrodes of Pt-based materials doped with small and different Au contents on 8% mol Y 2 O 3 -stabilized ZrO 2 (8YSZ) solid electrolyte substrates by screen printing and high-temperature co-firing. The effects of Au on the porous Pt electrode’s catalytic activity and long-term stability were investigated, and the results are as follows. First, the catalytic capacity of the Pt–Au alloy electrode decreases with increasing Au content due to the inhibition of the oxygen adsorption on Au, which decreases the amount of oxygen participating in the reaction at triple-phase boundaries (TPBs). Second, the catalytic ability of the alloy electrode decreases exponentially with aging time due to the reduction in the length of TPBs caused by the significant reduction in the number of holes in the electrode, and the oxidation of Pt. In addition, the conductivity decay rate of the electrode decreases with increasing Au doping. This indicates that Pt-based electrodes doped with varying Au contents, long-term, and high-temperature aging have notably regular effects on the catalytic activity of oxygen-pumping electrodes, for which we have developed a model of Au passivation and the synergistic effect of aging time on the activity of Pt-based oxygen-pumping electrodes.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Lin An,Yuxi Jia,Jinran Li,Chunsheng Xiao
Melanoma, the deadliest skin cancer with high metastasis potential, has posed a great threat to human health. Accordingly, early efficient blocking of melanoma progression is vital in antitumor treatment. Herein, a reduction-responsive dextran-based Pt(IV) nano-prodrug (PDPN) was synthesized and used for doxorubicin (DOX) delivery to combat melanoma synergistically. First, PDPN was prepared by one-pot chemical coupling of carboxylated methoxy poly(ethylene glycol) (mPEG), dextran (Dex), and the crosslinking agent cisPt (IV)-COOH. PDPN had a spherical structure ( R h = 34 ± 11.3 nm). Then, DOX was encapsulated into the PDPN core to form DOX-loaded PDPN (PDPN-DOX). The obtained PDPN-DOX displayed reduction-responsive release of DOX and Pt, thus showing a synergistic anticancer effect in B16F10 cells (combination index, 0.46). Furthermore, in vivo experiments demonstrated that PDPN-DOX was effective for the synergistic treatment of subcutaneous melanoma. Collectively, the as-prepared PDPN could serve as a promising and versatile nano-prodrug carrier for the co-delivery of chemotherapeutics in tumor combination therapy.
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Analytical Methods
·
2022
·Vol. 14
·期 48
·5091-5099
·
IF 3.532
Yue Sun,Zihao Xie,Fubin Pei,Wei Hu,Shasha Feng,Qingli Hao,Bing Liu,Xihui Mu,Wu Lei,Zhaoyang Tong
The rapid spread of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) seriously threatened global public health. Establishing a rapid and sensitive diagnostic test for early detection of the SARS-CoV-2 nucleocapsid protein is urgently required to defend against the pandemic. Herein, an enhanced lateral flow immunoassay (LFIA) was fabricated by trimetallic Au@Pd@Pt core–shell nanozymes for detection of the SARS-CoV-2 nucleocapsid protein. The Au@Pd@Pt nanozymes (Au@Pd@Pt NZs) synthesized via a one-pot method, with a dendrite morphology and uniform particle size, showed excellent peroxidase-like activity. Due to the perfect enzyme-like catalytic activity toward 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H2O2), the catalytic signal could be generated even by a tiny amount of Au@Pd@Pt NZs accumulated on the test strip. Therefore, rapid detection with higher sensitivity was achieved. The Au@Pd@Pt NZs-based LFIA provided a quantitative range of 0.05–100 ng mL−1 with a limit of detection of 0.037 ng mL−1, which was 17-fold lower than the LFIA without enhancement. The average recoveries from spiked samples were in the range of 92.5–107.9% with relative standard deviations all less than 4%, indicating the reliability and repeatability of the proposed LFIA. Additionally, the proposed LFIA could report results within 30 min using a microplate reader. In conclusion, the Au@Pd@Pt NZs-LFIA is a rapid, simple, and sensitive method for detecting the SARS-CoV-2 nucleocapsid protein.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Fuyuan Sun,Ruifa Su,Yingyu Zhou,Hongfeng Li,Fanchen Meng,Yongqi Luo,Shiming Zhang,Weina Zhang,Baoli Zha,Suoying Zhang,Fengwei Huo
High-loading Pt/C catalysts play an important role in the practical application of metal–air batteries and fuel cells because of their superior activity, high conductivity, and commercial availability. It is well known that high loadings always lead to the agglomeration of Pt nanoparticles, resulting in a loss of catalytic activity and stability; thus, it still remains a challenge to prepare high-loading Pt/C catalysts with high dispersion and small particle sizes. Here, we introduce a surfactant-assisted microwave discharge method to prepare high-loading (>40 wt %) Pt/C electrocatalysts with ultrafine particle sizes (∼3.19 nm) and good dispersion. Benefitting from the high-temperature property and reducibility of carbon-induced-arc, the surfactant and Pt precursors undergo rapid decomposition, reduction, and carbonization, generating the structure of Pt@C on carbon black. The carbon derived from the surfactant can not only inhibit the agglomeration of Pt nanoparticles but also prevent the Pt core from toxication, ensuring high activity and stability of the high-loading Pt/C catalyst. When evaluated in the oxygen reduction reaction, the as-prepared Pt/C catalyst demonstrates a comparable activity and better methanol resistance to commercial Pt/C.
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Frontiers in Chemistry
·
2022
·
IF 5.545
Wang Yaju,Zhou Zhiming,Wang Chao,Zhao Leihong,Xia Qineng
The selective hydrogenolysis of glycerol to 1,3-propanediol (1,3-PDO) with high added value is attraction but challenging. Pt-WOx-based catalysts have been extensively studied in the selective hydrogenolysis of glycerol. The catalyst support and the physicochemical state of WOx play important roles on this reaction. In this paper, Pt-WOx catalysts supported on TiO2 with different crystal forms were prepared and studied for their catalytic performance in hydrogenolysis of glycerol. It was observed that the catalytic performance of anatase-type (A-type) TiO2-supported catalyst (Pt/W/A-Ti) is much better than that of the rutile-type (R-type) TiO2 catalyst (Pt/W/R-Ti) due to its higher stability. Furthermore, the influence of W loading amount and state were thoroughly investigated for the Pt/W/A-Ti catalysts, and Pt/W/A-TiO2 with 5 wt% loading of WOx achieved the best catalytic performance (100% conversion of glycerol and 41% yield of 1,3-PDO under the optimal reaction conditions), owing to the suitable WOx domains and high dispersion of W species, as evidenced by XRD patterns and TEM images. Mechanism study by in-situ DRIFTS experiments indicated that glycerol was first converted to 3-hydroxypropanal and then converted to 1,3-PDO through subsequent reactions.
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