Chem Catalysis
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2023
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IF 9.4
Zhongliang Huang,Siyuan Hu,Yinan Xu,Jinxin He,Dongren Cai,Kang Sun,Jianchun Jiang,Guowu Zhan
Summary The interfacial sites of metal-support catalysts are crucial for catalytic reactions. Herein, we designed well-defined N-Co 3 O 4 /Pt catalysts with N-tailoring metal-support interfaces to promote catalytic activity toward CO oxidation under humid environments. A series of N-Co 3 O 4 /Pt catalysts were fabricated using ZIF-67 nanocubes as self-sacrificing templates, which showed exceptionally high catalytic activity in low-temperature CO oxidation. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study indicates that H 2 O molecules undergo dissociative adsorption to form active –OH species (Co 3+ –OH–Pt). Isotopic labeling technique indicates that H 2 O molecules (or –OH groups) contribute to ∼65% of CO 2 production in CO oxidation. Moreover, the amount of N dopant that stabilized the Co 3+ –OH–Pt species was highly dependent on the H 2 O-soaking conditions of ZIF-67/Pt. Density functional theory (DFT) calculations suggest that the COOH ∗ pathway of CO oxidation over the N-Co 3 O 4 /Pt interface is energetically favorable in humid conditions. In particular, the N doping could stabilize the Co 3+ –OH–Pt interface and simultaneously reduce the energy barrier of CO 2 formation from COOH ∗ intermediates.
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TALANTA
·
2023
·
IF 6.1
Jie Liu,Zixuan Zhang,Jie Dong,Anyi Chen,Jingfu Qiu,Chaorui Li
As a reliable biomarker to evaluate the severity of sepsis, sensitive and accurate detection of procalcitonin (PCT) is essential. In this study, a dual-mode electrochemical immunosensor based on Au/ZIF-8 as substrate and Pt@Cu 2 O as signal label was constructed for the detection of PCT. By loading Au nanoparticles onto rhombic dodecahedral ZIF-8, the substrate (Au/ZIF-8) has large specific surface area and can immobilize antibody (Ab 1 ) by Au–N bonds. Meanwhile, hollow Pt@Cu 2 O nanocomposite with excellent peroxidase-like activity and electrocatalytic activity were synthesized as signal label. In the process of electrochemical testing, Pt@Cu 2 O catalyzed the reduction of hydrogen peroxide (H 2 O 2 ) and further promotes the oxidation of hydroquinone (HQ) to achieve the synergistic amplification of electrochemical signals. The proposed immunosensor detected PCT by amperometric i-t and differential pulse voltammetry (DPV) tests with a good linear response and low limit of detection (i-t: 0.70 fg/mL and DPV: 0.40 fg/mL) in the range of 10 fg/mL∼100 ng/mL. The immunosensor exhibited excellent sensitivity and accuracy, indicating the potential application of this method for PCT detection.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Shaobin Li,Jingwei Liang,Xiaoguo Tan,Fengbo Li,Xinming Wang,Lin Ma,Li Zhang,Kun Cheng
Electrochemical water splitting is regarded as a promising technology for production of high purity, high volume hydrogen. It is critical to create robust and highly active electrocatalysts in order to minimize the cost of hydrogen generation and enable large-scale commercial production. In this work, a new 2D MoCu-POMOF, [Cu(4-pyz)] 4 @(PMo 12 O 40 ) (4-pyz = 4-(pyridin-4-yl)benzoic acid) was prepared by a simple hydrothermal method , in which PMo 12 nanocluster was encapsulated into cavity of 2D Cu-MOF. The successful establishment of the model in addition to the goal of uniformly dispersed Mo sources target oxygen-rich PMo 12 nanoclusters can also provide rich Mo source and self-oxidative properties for MoO 2 formation. Cu-MOF provides a special layered structure, which ensures the integrity and stability of the structure and provides a rich C source for pyrolysis and improves the conductivity. Ultralow Pt nanoparticles can reduce free energy of hydrogen evolution , which are embedded in MoO 2 /MoOC with porous structure and high electrochemical active surface area . MoO 2 /MoOC and highly dispersed Pt nanoparticles synergistically promote the HER catalysis. Pt@MoO 2 /MoOC demonstrated the excellent HER activity with a low overpotential of 98.99 mV vs. RHE. This work yielded highly active and high stability molybdenum-based HER electrocatalysis and provides the potential for energy conversion.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Qiuyu Shen,Zhihui Lu,Fukun Bi,Dongfeng Zhang,Lijuan Li,Xiaodong Zhang,Yiqiong Yang,Minghong Wu
The synthesis method of precious metal catalysts would affect the electronic metal-support interaction (EMSI) of catalysts, which further affected the catalytic activity. In this paper, Co 3 O 4 was obtained as support by the pyrolysis of ZIF-67 as a template sacrificial agent, and Pt species were loaded by three different reduction methods. Among them, the catalyst produced by the NaBH 4 reduction method possessed the best activity with T 90 of 168 °C. Through a series of characterization and experiments, it was found that the EMSI of the catalyst was optimized by this synthesis method, which led to electron transfer among Pt species and Co 3 O 4 . The catalysts also exhibited excellent water resistance, stability, and recycling performance. The possible degradation mechanism of toluene was also revealed by in situ DRIFTS and GC–MS. This paper provided ideas for the construction of catalysts and a theoretical reference for the relevant verification of EMSI.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xiaoling Liu,Yitong Liu,Yue Wu,Shan Dong,Guoqin Qi,Cailing Chen,Shibo Xi,Pan Luo,Yihu Dai,Yu Han,Yu Zhou,Yu Guo,Jun Wang
Catalytic oxidation of volatile organic compounds like formaldehyde (HCHO) over the noble metals catalysts at room temperature is among the most promising strategies to control indoor pollution but remains one challenge to maximize the efficiency of noble metal species. Herein, we demonstrated the straightforward encapsulation of highly dispersive Pt nanoparticles (NPs) within BEA zeolite and adjacent with the surface hydroxyl groups to reach the synergistic HCHO oxidation at 25 °C. High efficiency and long-term stability was reached under large space velocity (∼100% conversion at 180,000 mL (g cat × h) −1 and >95% at 360,000 mL (g cat × h) −1 ), affording rapid elimination rate of 129.4 μmol (g Pt × s) −1 and large turnover frequency of 2.5 × 10 −2 s −1 . This is the first synergy example derived from the hydroxyl groups and confined noble metals within zeolites that accelerated the rate-determining step, the formate transformation, in the HCHO elimination.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Minglu Wang,Ying Wang,Xiangyang Li,Hongyan Zhang
The continuous intake of diethylstilbestrol (DES) residue seriously threatens the health of consumers, so the rapid and sensitive detection of DES is helpful for timely food safety warning. In this study, a photothermal-sensing microfluidic paper-based analytical chip (PT-Chip) was developed for effectively screening of DES residue in foods. Competitive inhibition immunochromatography was introduced and the composite of black phosphorus nanosheets and gold nanoparticles (BP-Au) was used as signal indicators. Then, the test area was irradiated by an 808 nm laser and the photothermal transduction signal was recorded by a thermal imager to achieve sensitive photothermal detection. The amount of DES was obtained by analyzing the temperature change curve of test area. The PT-Chip can achieve accurate quantification of DES with a detection limit of 0.1 μg/L. And the successful determination of DES in different food samples indicating that the PT-Chip can be used as a promising detection device.
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ACS Catalysis
·
2022
·
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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Haoyang Fu,Meirong Li,Qianyu Xu,Guoliang Chen,Yunjie Zou,Weixian Zhang,Shuzhou Li,Lan Ling
Downsizing supported metal of Fe 0 -based materials in dealing with ever-growing pharmaceutical contamination issues are highly desired but still challenging. Herein, we develop a modular design protocol to synthesize a family of ultrafine alloy nanoclusters embedded in a nitrogen-enriched carbon framework (NEC@FeM (M=Pd, Pt, Au)). Engineering the fine structure of nitrogen-enriched carbon and interfacial interaction with bimetallic nanoclusters largely suppresses bimetallic overgrowth, eventually producing supported ultrafine (< 4 nm), highly dispersed, well-alloyed nanoclusters. The alloying Fe 0 with M for ultrafine nanoclusters optimize the electron flow, chemical stability, and catalytic property, resulting in the obtained NEC@FeM exhibiting excellent doxorubicin (DOX) degradation performance. Density functional theory calculation combined with experimental results attribute the outstanding DOX degradation ability of NEC@FePd originally to the synergistic effect of enhanced DOX affinity and efficient electrons transfer from Fe to DOX. This work provides a paradigm for the design of ultrafine Fe 0 -based nanocluster with application in pollution control.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
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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Frontiers in Materials
·
2022
·
IF 3.985
Pei Mengxi,Lv Shangchun,Liu Yishui,Si Zhichun,Wu Xiaodong,Ran Rui,Weng Duan,Kang Feiyu
Photocatalytic removal of organic pollutants under solar irradiation at room temperature is considered an energy-saving technique of environmental remediation. However, photocatalysis is impeded by the poor response to visible light and fast charge recombination. In this work, sub-nano Pt/β-FeOOH quantum dots (QDs) were designed to shorten the charge migration path and obtain wide light harvesting. Interestingly, the crystalline β-FeOOH QDs can be obtained by loading sub-nano Pt particles via a reconstruction mechanism of amorphous FeOOH induced by H2 spillover, which facilitates the fast kinetics of charge transition and benefits the oxygen-rich surface of the catalyst for photocatalytic oxidation reactions. Moreover, the Pt-VO-Fe interfaces were proved to be the most active sites for the activation of O2. As a result, the catalyst exhibits a predominant photocatalytic performance in toluene oxidation, achieving a TOFPt of 0.591 min−1 at room temperature under visible light irradiation. This work provides a new perspective on the design and preparation of nanocatalysts for high-efficient photocatalysis under visible light irradiation.
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Advanced Materials Interfaces
·
2022
·Vol. 9
·期 26
·2201263
·
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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Yangjun Luo,Yanwei Wang,Youyuan Wang,Heming Huang,Li Zhang,Huijuan Zhang,Yu Wang
Although various alloys have been extensively explored to enhance catalyst activity and stability in oxygen reduction, degradation of performance due to long-term operation has plagued the crowd. Here, we develop a catalyst synthesis strategy based on the coexistence of monoatomic Fe and Pt-based clusters/alloys on NC/TiO x . Fe/PtCo-NC/TiO x exhibits a half-wave potential of 0.948 V and mass activity of 3.69 A mg Pt −1 at 0.9 V, the latter being approximately 32.1 times higher than that of 20% Pt/C (0.115 A mg Pt −1 ). Additionally, it also shows maximum power densities of 952.2 mW cm −2 and 215.8 mW cm −2 in the H 2 /O 2 fuel cell and Zn-air battery, respectively. The combination of illumination and calcination promotes the electron transfer between Pt and TiO x , thus enhancing the catalytic activity and stability. We also explore the approach and mechanism of using illumination to suppress catalyst performance degradation. The intermittent irradiation inhibits the dissolution of Pt to facilitate the Fe/PtCo-NC/TiO x durability beyond that of most reported metal catalysts, with a half-wave potential degradation of only 14 mV after 30,000 cycles. The ingenious use of illumination provides a simple and feasible strategy for the sustainable utilization of catalysts.
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