CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jian Tian,Chuanhu Wang,Junwei Wu,Daohua Sun,Qingbiao Li
Pt works particularly well as a nanoparticle catalyst in the elimination of atmospheric pollutants, but its application is severely hampered by agglomeration and even poisoning in the presence of moisture. Hereby, a novel catalyst Pt@O-ZSM-5@OTS was synthesized to protect Pt, namely 0.5 wt% Pt was integrated into hollow ZSM-5 and subsequently coated hydrophobic octadecyltrichlorosilane (OTS) akin to the waterproof carapace. With the aid of various characterization techniques, the hybrid catalyst induced multiple marked features, such as dual-shell structure, hydrophobic microenvironment, and encapsulated active sites. Under excessively humid conditions (10 vol% H 2 O), the optimized Pt@O-ZSM-5@OTS2 exhibited a stable benzene conversion efficiency of 100 % for 120 h and outperformed the catalysts reported so far. Even reducing the reaction temperature to 170 °C, the conversion of benzene also reached 85 %, far exceeding the performance of untreated Pt@O-ZSM-5 (∼50 %). The outstanding stability stems from the hollow structure and OTS shell, which not only provide Pt with a protective shield against active site coverage, but also enhance competitive adsorption to benzene. Furthermore, DFT simulations unveil that the hydrophobic OTS shell enhances water resistance, consequently facilitates the oxidative degradation of contaminants at the active site. This work sheds light on novel strategies for the preservation of Pt by hydrophobic zeolite structures, as well as a deeper understanding of the elimination of aqueous VOCs.
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ACS Catalysis
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2022
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IF 13.7
Weiyue Zhao,Bin Chi,Lecheng Liang,Pengfei Yang,Wei Zhang,Xin Ge,Liming Wang,Zhiming Cui,Shijun Liao
Developing advanced electrocatalysts toward the sluggish oxygen reduction reaction (ORR) kinetics is critical to fuel cells but still an enormous challenge at present. Here, we demonstrate a highly active and durable Pt-based ternary catalyst, ordered Pt3Co0.6Ti0.4 intermetallic nanoparticles (∼3 nm) supported on ZIF-8-derived mesoporous carbon (Pt3Co0.6Ti0.4/DMC). The Pt3Co0.6Ti0.4/DMC catalyst exhibits faster ORR kinetics compared to Pt3Co/DMC and commercial Pt/C with minimal activity loss (20.1%) and only 5 mV decay in half-wave potential after 20,000 potential cycles. More importantly, its improved performances have also been proven in the H2/air PEM single cell test. The theoretical calculations reveal that the substitution of Ti for Co induces a strengthened ligand effect and optimizes the surface electronic structure of Pt3Co0.6Ti0.4, resulting in the significantly enhanced ORR activity. This work provides a reliable and promising approach for the development of efficient and robust Pt-based ternary intermetallic electrocatalysts for practical fuel cell applications.
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Advanced Materials Interfaces
·
2022
·Vol. 9
·期 26
·2201263
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IF 6.389
Mingan Zhou,Minghao Liu,Qiyang Miao,Hengfu Shui,Qing Xu
Oxygen reduction reaction (ORR) plays key roles in fuel cells and metal air batteries. Covalent organic frameworks (COFs)-derived carbons have been utilized for catalyzing ORR. However, the activity and selectivity for these catalysts in the acidic medium is still under improved. In this work, Pt atoms and uniform Pt nanoparticles supported by standing carbons are derived from a three-dimensional COF. With increasing the contents of Pt ions, the corresponding particle sizes show obvious decrease, and thus resulting in higher catalytic activity. The synergetic roles between Pt atoms and nanoparticles with average sizes of 6.19 nm make catalyst show remarkable activity toward ORR, with onset potential and half-wave potential of 0.98 and 0.85 V (vs RHE) in the acidic medium, which are 70 and 40 mV more positive than those of Pt/C, respectively. This work provides a new insight for developing COFs in energy storage and conversion systems.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Binbin Zhao,Yu Liang,Wenjun Yan,Lei Liu,Jinxiang Dong
Selective hydrogenolysis of biomass-derived glycerol to 1,3-propanediol (1,3-PDO) is of significant industrial value. The conventional synthetic approach for the supported Pt–WOx catalysts with potential for industrial application generally required a high Pt loading with an aim to create more Pt–O–W interfaces owing to the difficulty in controlling the formation of active WOx species and their high dispersion on supports. In this study, a thin coating of a WOx–Ta2O5 solid solution on a Ta2O5 surface was successfully fabricated by the calcination of W-precursor-containing Ta2O5 at a high temperature (i.e., 900 °C), leading to high dispersion of low-polymeric tungsten oxide with abundant oxygen defects on the support surface. The oxygen defects of the WOx species in the WOx–Ta2O5 solid solution layer played a key role in anchoring and dispersing platinum species to maximize the Pt–O–W interface. WOx(900)/Ta2O5-supported Pt exhibits much higher catalytic efficiency toward the production of 1,3-PDO (TOF1,3-PDO = 23.2 g1,3-PDO·gPt–1·h–1) than that of WOx(500)/Ta2O5-containing Pt derived from routine calcination temperatures. Several characterization techniques were applied to examine the state change of WOx on the support by varying the calcination temperature, as well as the effect of WOx species on the dispersion and chemical states of platinum species.
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CHEMOSPHERE
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2021
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IF 7.086
Jian Tian,Kok Bing Tan,Yichen Liao,Daohua Sun,Qingbiao Li
A zeolitic cage was introduced and rationally fabricated by encapsulating Pt nanoparticles (NPs) in hollow ZSM-5, a nanomaterial with a cavity and porous shell, for efficient catalytic oxidation of benzene. The structure and formation of the zeolitic cage were systematically investigated and characterized using transmission electron microscopy , nitrogen sorption investigations, X-ray photoelectron spectroscopy, nuclear magnetic resonance spectroscopy , and X-ray diffraction. The obtained hollow 0.2 Pt@ZSM-5 exhibited a comparable low-temperature catalytic activity with 0.5Pt/ZSM-5 with T 90 value of 178 °C. Various characterization techniques combined with adsorption experiments uncover the tremendous role of the zeolitic cage in the catalytic activity toward benzene oxidation. The porous shell prevented benzene dilution and the acidity originating from the hollow interior of ZSM-5 promoted the storage of benzene, thereby forming a high local concentration of benzene around Pt NPs, resulting in excellent catalytic performance. These findings provide valuable insights into the rational design of efficient catalysts for the catalytic oxidation of volatile organic compounds.
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PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2021
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IF 5.455
Jipeng Meng,Di Bai,Pahaer Zeyaodong,Chuang Li,Xiao Chen,Changhai Liang
The wirelike, rodlike and corolla-like ZSM-48 zeolites with various SiO 2 /Al 2 O 3 ratios (SARs) were successfully synthesized and exploited for the hydroisomerization of n-hexadecane (n-C 16 ). The influences of metal-acid balance, acid sites quantity, crystal morphology and textural properties on n-C 16 hydroisomerization performance were investigated primarily, via various characterization technique such as XRD , FT-IR, SEM, TEM, N 2 physisorption , NH 3 -TPD, and Py-IR. The C Pt /C A ratios of various catalysts were calculated for the quantified expression of the metal-acid balance, and the acid sites quantity was seriously crucial for the consecutive acid-catalyzed reaction after C Pt /C A ratios satisfied within an ideal range. Large external surface could accelerate the conversion rate, shorten the diffusional constraints and inhibit the cracking. The superiorities of satisfied C Pt /C A values (0.12–0.15), high concentration of acid sites (>230 μmol/g) and large external surface (>120 m 2 /g) persuaded the Pt/Z(P)80, Pt/Z(H)60 and Pt/Z(H)80 samples to demonstrate wonderful hydroisomerization performance with outstanding yield around 80 wt% and excellent i-C 16 selectivity over 91 wt%. Although Pt/Z(W)80 and Pt/Z(R)80 samples owned the relatively small crystal, the gloomy catalytic activity of them was observed due to their relatively low concentration of acid sites and external surface. Moreover, the presence of “key-lock” mechanism was verified by the observations of 7-methyl-pentadecane (7MC15) dominating in isomer products.
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BIOELECTROCHEMISTRY
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2021
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IF 5.373
Fenglin Zhang,Zhiguang Liu,Yujie Han,Lifang Fan,Yujing Guo
Carcinoembryonic antigen (CEA) is considered as a disease biomarker, which is related to various cancers and tumors in the human bodies. Sensitive detection of CEA is significant for clinical diagnosis and treatment. Herein, we proposed an electrochemical aptasensor for CEA detection based on the amplification driven by polydopamine functional graphene and Pd-Pt nanodendrites ( [email protected] /Pd-PtNDs), conjugated hemin/G-quadruplex (hemin/G4), which possess mimicking peroxidases activity. Firstly, [email protected] was modified on the electrode surface for fixing CEA aptamer 1 (Apt1). Then, [email protected] /Pd-PtNDs with large surface area served as matrix for immobilization of hemin/G4 to obtain the secondary aptamer. In virtue of the sandwich-type specific reaction between CEA and the corresponding aptamers, the second aptamer was captured on the sensing interface, which can catalyze the oxidation of signal probe hydroquinone (HQ) with H 2 O 2 and amplify current signal. Furthermore, the electrochemical signals of HQ were proportional with CEA concentrations. Under the optimal conditions, a dynamic response range from 50 pg/mL to 1.0 μg/mL and a detection limit of 6.3 pg/mL for CEA were obtained. Moreover, the proposed strategy represented satisfactory sensitivity and stability, and showed a good precision in real samples application.
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Materials Today Energy
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2021
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IF 7.311
Xilong Wang,Yadong Li,Chen Yang,Jiajia Lu,Lijuan Cao,Han-Pu Liang
A considerable number of strategies have been investigated to construct highly-efficient and stable Pt-based electrocatalysts for promoting the oxygen reduction reaction, which plays a critical role in proton exchange membrane fuel cells and metal-air batteries. In this contribution, Pt-based intermetallic nanoparticles confined in a Co-doped zeolitic imidazolate framework-8 derived carbon matrix with cobalt nanocrystallites and Co-N x sites decoration are conceptually predicted and experimentally constructed by a novel surfactant-assisted Pt implantation and in-situ alloying strategy. Cationic surfactant cetyltrimethylammonium bromide was simultaneously used as the functional capping ligand to coordinate with [PtCl 6 ] 2- and structure-directing agent for synthesis of rod-like Co-doped zeolitic imidazolate framework-8. Systematical characterization and contrast experiments reveal that the Pt-based intermetallic compounds are mainly Pt 3 Co nanocrystalline , and cetyltrimethylammonium bromide is critically important for Pt reservation and highly dispersion in the resulting electrocatalyst. The as-synthesized Pt 3 Co/Co@Co–N–C electrocatalyst with a low Pt content (∼7 wt%) shows a positive half-wave potential of 0.922 V and a high limiting current density of ∼6 mA cm −2 . More importantly, compared with commercial Pt/C, Pt 3 Co/Co@Co–N–C features high stability with mass activity increased from 362 mA/mg Pt to 400 mA/mg Pt after 30,000 voltage cycles from 0.6 to 0.9 V vs. reversible hydrogen electrode. The strategy for the construction of oxygen reduction reaction electrocatalyst with Pt and transition metal-doped catalysts provides a new opportunity to design advanced hybrid catalysts for various electrocatalysis processes.
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Journal of Physical Chemistry C
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2021
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IF 4.126
Chen Ding,Zijie Mao,Jia-Shun Liang,Xianxian Qin,Qing Zhang,Fan Yang,Qing Li,Wen-Bin Cai
The commercialization of proton exchange membrane fuel cells (PEMFCs) calls for the development of active and durable Pt-based catalysts for oxygen reduction reaction (ORR) by means of a cost-effective and environmentally benign protocol. We report herein an all aqueous phase preparation of carbon supported Au-modified Pt–Co alloy catalyst (Au/Pt–Co/C), which involves the dimethylamine borane co-reduction of aqueous Pt(II) and Co(II) precursors to form a Pt–Co/C catalyst and the ethanol reduction of an aqueous Au(III) precursor to form Au/Pt–Co/C. This Au/Pt–Co/C catalyst not only shows a greatly enhanced ORR activity like the homemade Pt–Co/C and state-of-art Pt–Co/C(com) catalysts as compared to the Pt/C catalyst but also exhibits a much higher durability over the Pt/C(com), homemade Pt–Co/C, and state-of-art Pt–Co/C(com) catalysts in accelerated degradation tests (ADTs) with both half-cell and single-cell configurations. Specifically, the maximum power density of a PEMFC involving the Au/Pt–Co/C cathode suffers only a 6% loss after 30 000 cycles of a standard ADT while that involving the state-of-art Pt–Co/C(com) suffers a 37% loss. This research provides an alternative route to prepare efficient and durable Pt-based ORR catalysts toward a widespread application of PEMFCs.
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Journal of Materials Chemistry A
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2021
·Vol. 9
·期 22
·13080-13086
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IF 12.732
Mei Zhang,You Xu,Shengqi Wang,Mengying Liu,Lianbang Wang,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
How to boost the electrocatalytic performance of non-Pt catalysts for the hydrogen evolution reaction (HER) to substitute Pt is an important research topic. Herein, by combining a one-pot wet-chemical method and the post surface functionalization, we successfully fabricated polyethylenimine (PEI)-modified bimetallic Au@Rh core–shell mesoporous nanospheres (Au@Rh@PEI MNs). Benefiting from the synergetic effects of Au@Rh core–shell mesoporous architectures and interfacial modification by PEI molecules, the resultant Au@Rh@PEI MNs exhibit excellent electrocatalytic activity and stability for the HER in all pH value solutions, which even surpass the benchmark commercial Pt/C catalyst. Our synthetic protocol may offer guidelines for the rational design of advanced catalysts for water splitting and other electrocatalytic applications.
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SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Chaozhu Huang,Jingwei Zhao,Fengdong Qu,Jiacheng Wang,Minghui Yang
Hydrogen sulfide (H 2 S) is considered a highly hazardous toxic gas. H 2 S sensors are therefore of paramount significance for real-time leak detection. However, existing solutions do not meet the strict performance targets set by stakeholders, while deactivation due to surface area of sensing materials decrease and contamination is a widely unsolved problem. Presented here is a new support material, mesoporous niobium nitride (NbN), which improve the long-term stability largely via enhancing the interaction between metal and support. Simultaneously, sensor devices using NbN as support show enlarged sensitivity, enhanced limit of detection and well repeatability when compared with these sensors using traditional carbon black support. In a wider perspective, our work suggests strategies for enhancing long-stability of next-generation chemical gas sensors by optimizing metal-support interaction.
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 23
·10315-10324
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IF 3.591
Jianming Fan,Jinhua Xiong,Dayue Liu,Yuanping Tang,Song He,Zhibiao Hu
A novel strategy was developed to fabricate a CdS/Pt photocatalyst (defined as CdS/w%Pt-PAR) via the cathodic photocorrosion effect of CdS. A tentative mechanism for Pt deposition on CdS via the cathodic photocorrosion effect was proposed, based on a series of electrochemical characterization methods, such as cyclic voltammetry and Mott-Schottky tests. Transmission electron microscopy verified that Pt was grafted on the CdS surface via a heterojunction. Moreover, a strong interaction between Pt and CdS was further confirmed by X-ray photoelectron spectroscopy. The optimal photocatalytic H2 evolution rate of CdS/2%Pt-PAR was 1086.1 μmol h−1, 6.4 and 2.6 fold higher than that of the reference samples synthesized by traditional photodeposition (CdS/2%Pt-PD) and chemical reduction (CdS/2%Pt-CR) methods, respectively. Linear sweep voltammetry and fluorescence experiments verified that CdS/2%Pt-PAR has a lower H2 evolution overpotential and faster separation of photogenerated carriers, respectively, compared with CdS/2%Pt-PD and CdS/2%Pt-CR. This work paves a new route for fabricating CdS/metal photocatalysts with highly efficient and stable photocatalytic H2 evolution activity.
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