Journal of Physical Chemistry C
·
2015
·
IF 4.772
Shan Wang,Guang Yang,Shengchun Yang
PtNi3 bimetallic concave octahedrons with a majority of platinum atoms deposited on the frames were synthesized in ethylene glycol solution. The high angle annular dark field scanning transmission electron microscopy (HAAD-STEM) characterizations and energy-dispersive X-ray spectroscopy (EDS) analysis reveal that the Pt frames have a thickness of less than 2 nm, which surround a nickel core thus forming a quasi core–shell concave octahedral nanoparticle (NP). The element-specific anisotropic growth followed by the nanoscale phase segregation and subsequent oxidation of Ni riched facets are responsible for the formation of the concave nanostructure. The PtNi3quasi core–shell concave octahedrons exhibit substantially enhanced electrocatalytic properties toward methanol oxidation and hydrogen evolution reaction compared with that of the commercial Pt/C, suggesting that the Ni riched Pt–Ni NPs can be used as a potential candidate for methanol oxidation reaction (MOR) or hydrogen evolution reaction (HER) catalysts with the low utilization of Pt.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jinglei Cui,Yujun Cui,Jingjing Tan,Huirong Zhang,Mengyuan Gu,Long Huang
Volatile organic compounds (VOCs) are one of the main pollutants produced in industrial processes. Catalytic oxidation is an effective method to eliminate VOCs, and the key lies in designing efficient metal catalyst. In this work, Pd-Pt/SiO 2 bimetallic catalysts were designed and prepared by the immobilization method, and their performances for toluene oxidation were evaluated. The addition of Pt into the catalyst elevated markedly the reduction of Pd active sites, leading to abundant electron-deficient Pd 0 and electron-rich Pt 0 in the Pd 2 Pt 1 catalyst, which were confirmed by TEM, CO pulse adsorption and in-situ XPS. As revealed by O 2 -TPD and toluene-TPD characterization, the cooperative effect of electron-deficient Pd 0 and electron-rich Pt 0 in Pd 2 Pt 1 catalyst facilitated the activation of O 2 and toluene, thus enhanced greatly its activity. A conversion of 90% (T 90 ) for toluene was achieved over Pd 2 Pt 1 catalyst at 165 ℃, and the apparent activation energy ( E a ) over Pd 2 Pt 1 catalyst was lower than that over other Pd-Pt bimetallic and monometallic Pd or Pt catalysts. Additionally, the reaction mechanism was studied by In - situ DRIFTS, the results showed that the toluene oxidation passed successively benzyl alcohol, benzaldehyde, benzoic acid and maleic anhydride , then maleic anhydride was further oxidized to CO 2 and water.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Jiang-Hao Lu,Ze Li,Di Zhang,Lu-Hang Song,Xiao-Yan Cai,Liang Mao,Zhi-Qiang Liu,Zhi-Jie Wang,Xiu-Quan Gu,Guo-Dong Yuan
The nano/microstructuring of silicon (Si) via chemical methods has garnered significant attention due to its excellent light-trapping capabilities across a wide spectral range. Current research has predominantly focused on the synthesis of pyramidal-shaped microtextures, which enable two reflections on the surface, while largely overlooking the superior light-trapping potential of inverted pyramid silicon (SiIP) microtextures, which theoretically allow for three reflections. Moreover, there has been limited investigation into the application of inverted pyramid black silicon for solar-driven hydrogen evolution. This study reports the synthesis of uniformly arranged inverted pyramid-textured black silicon using the copper-assisted chemical etching (Cu-ACE) method to enhance the efficiency of solar-driven water splitting for hydrogen production. The formation mechanism and the influence of copper-localized surface plasmon resonance (Cu-LSPR) from Cu nanoparticle (NP) byproducts on photoelectrochemical (PEC) activity were systematically analyzed. To reduce sidewall defects and minimize photogenerated carrier recombination, the surface of the SiIP was treated with tetramethylammonium hydroxide (TMAH). A vertical PN junction was developed through ion implantation to reduce the external bias of the SiIP. Additionally, a uniform TiO₂ antireflective layer was deposited via atomic layer deposition (ALD), reducing the average reflectance of the SiIP-T 4 to 5.78 % over the 300–1100 nm wavelength range. MoSₓ and Pt NPs were electrodeposited to improve the fill factor and enhance HER kinetics. With optimized catalyst loading, the n + p-SiIP-T 4 /TiO₂/Pt 80 mC electrode achieved a photocurrent density of 8.0 mA cm −2 at 0 V vs. RHE, an applied bias photon-to-current efficiency (ABPE) of 0.93 % at 0.24 V vs. RHE, and a double-layer capacitance (Cdl) of 91 μF cm −2 . The onset potential (Von) was positively shifted by ∼1.13 V to 0.49 V vs. RHE compared to a SiIP photocathode, and the photocathode operated continuously at 0 V vs. RHE for 27 h in an acidic electrolyte. These results demonstrate that SiIP has significant potential for PEC hydrogen evolution, with further performance optimization achievable through structural and surface engineering.
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MOLECULES
·
2025
·Vol. 30
·期 3
·697
·
IF 4.6
Fukun Bi,Yaofei Zhang,Zhuoxuan Zhou,Lei Guo,Ziqiao Zhu,Baolin Liu,Xiaodong Zhang
Phthalic acid esters (PAEs), ubiquitous semi-volatile organic compounds (SVOCs) in indoor environments, pose adverse effects on human health. However, their degradation mechanisms and pathways remain unclear. Herein, we developed an efficient photothermal catalyst by introducing defects (oxygen vacancies, OVs) on TiO2(P25) surfaces via electron beam irradiation technology with different irradiation doses (100, 300, 500, and 700 kGy). The TiO2with defects was employed as a support to prepare Pt-TiO2catalysts for the photothermal degradation of di (2-ethylhexyl) phthalate (DEMP) and dimethyl phthalate (DMP), two representative PAEs. TiO2pre-treated with a 300 kGy irradiation dose supported the Pt catalyst (Pt-Ti-P-300) and presented the optimal catalytic performance for DEMP and DMP degradation. Characterization results confirmed that OVs were successfully introduced to the catalysts. Meanwhile, OVs induced by electron beam irradiation expanded the light absorption range and improved the generation and separation of photogenerated carriers, which significantly enhanced the catalytic activity of the catalysts for PAE degradation. Importantly, the degradation mechanism and pathway of DMP were further explored by using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and gas chromatography–mass spectrometry (GC-MS). These findings provide important insights into the electron beam irradiation-mediated regulation of catalysts and the photothermal catalytic removal of PAEs in indoor environments.
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PubMed
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Energy & Environmental Science
·
2024
·Vol. 17
·期 14
·5227-5240
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IF 32.4
Changle Yue,Chao Feng,Guangxun Sun,Na Liu,Haoyuan Hao,Wenjing Bao,Xiaowei Zhang,Fengyue Sun,Cong Zhang,Jiahui Bi,Yan Zhou,Hsiao-Chien Chen,Yuan Pan,Daofeng Sun,Yukun Lu
Tuning and stabilizing the chemical microenvironment of Pt-based single-atom catalysts is a major challenge in promoting an electrocatalytic hydrogen evolution reaction (HER). Herein, we constructed a hierarchical stabilization system of Pt single-atoms via defect substitution using the polyoxometalate (POM) (NH4)4[ZnMo6O24H6] (ZnMo6) as a template. The well-defined structure of ZnMo6 led to precise local Zn sublimation during the formation of Mo2C, which was converted from the Mo6 ring in situ. The localized defect provides a well-defined Mo(C)–Pt–N coordination environment to trap Pt single-atoms. The obtained single-atom catalyst (PtSA@Mo2C@NC) exhibited a superior and stable electrochemical HER performance with an unprecedented mass activity of 75.21 A mgPt−1 in 0.5 M H2SO4. In-depth theoretical calculation analysis revealed that Mo(C)–Pt–N coordination provides a moderated charge state and low d-band center of the Pt site, thus significantly promoting proton adsorption and H2 desorption. This work demonstrates a promising single-atom stabilization strategy for constructing high-performance HER electrocatalysts through the precise modulation of a three-dimensional chemical environment.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Nuo Zhang,Bingzhu Wang,Pengcheng Hu,Zhenxing Gao,Haiwang Wang
MCNTs-CdS has been identified as a promising material for photocatalytic hydrogen production due to its strong visible-light responsiveness and suitable energy band structure. However, the rapid complexation of its photogenerated electrons and holes makes its photocatalytic hydrogen production unsatisfactory. To address the above problem, MCNTs-CdS/Pt/ZnFe 2 O 4 composites were designed in this paper, and Pt was used as an electronic bridge to realize the fast transfer of electrons between the two semiconductors. The results show that the carrier transport resistance of MCNTs-CdS/Pt/ZnFe 2 O 4 system is greatly reduced, and the electron-hole separation rate is significantly better than that of MCNTs-CdS. In addition, the results of the photolysis of water hydrogen production demonstrated that when the deposition amount of Pt was 8 % and the mass ratio of MCNTs-CdS to ZnFe 2 O 4 was 1:0.1, the hydrogen production rate reached its maximum (1100.82 μmol/g/h), which was 35.51 times higher than that of MCNTs-CdS. The metal Pt functions as an electronic bridge to realize rapid electron transfer and MCNTs-CdS/Pt/ZnFe 2 O 4 form a Z-scheme carrier transport mechanism.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ruiqi Guo,Zhenglong Fan,Qiwei Zhou,Mengjie Ma,Wenxiang Zhu,Fan Liao,Hao Yang,Jiajie Wang,Zhenhui Kang,Minqi Sheng
Iridium oxide (IrO 2 ) has traditionally been considered to exhibit limited oxygen-reducing capacity. An effective approach to improve the oxygen reduction reaction (ORR) activity in parent catalytic materials is through atomic intercalation. However, the challenge lies in achieving a delicate balance between high ORR activity, structural stability, and minimizing the use of precious metals. Herein, we fabricate 3R-phase iridium oxide (3R-IrO 2 ) with superior ORR activity by intercalating a tiny amount of Pt (3.6 wt% Pt) into the interlayers of 3R-IrO 2 (3.6 wt% Pt-3R-IrO 2 ). When employed as an acidic ORR electrocatalyst, 3.6 wt% Pt-3R-IrO 2 shows a high half-wave potential (E 1/2 ) of 0.92 V (vs. RHE) in O 2 -saturated 0.1 M HClO 4 electrolyte, much better than those of Pt/C (0.850 V), 3R-IrO 2 (0.616 V), and Pt nanoparticles on 3R-IrO 2 surface (3.6 wt% Pt@3R-IrO 2 ) (0.618 V) electrocatalysts. It achieves high mass activity of 0.170 A mg Ir −1 at the potential of 0.9 V, which is 5.5 and 11.3 times than that of Pt/C (0.031 A mg Ir −1 ) and 3.6 wt% Pt@3R-IrO 2 (0.015 A mg Ir −1 ), respectively. Density functional theory (DFT) calculations and experiment results co-jointly demonstrate that the active center of Pt-3R-IrO 2 is anchored to the activated Ir atoms of the 3R-IrO 2 rather than Pt atoms. The d -band center of Ir 5 d orbitals of Pt-3R-IrO 2 is simultaneously regulated, which optimizes the energy barrier of adsorption/desorption toward the ORR process. Intriguingly, the intercalation of Pt atoms into trigonal rhodium oxide (Tri-RhO 2 ) also activates the ORR activity of Rh, suggesting the universality of this strategy. This discovery may provide a new and general way for activation of ORR activity of other precious metal-intercalated nonprecious metal oxide electrocatalysts.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Huiling Fan,Yuqi Qin,Long Li,Jiansheng Cui,Chenqiang Yang,Zhanhui Wang,Lili Duan,Yihong Wang,Liang Tian
Herein, a biosensing system was designed based on tripedal DNAzyme walker integrated nanoprobe signal amplification strategy for realizing ultrasensitive determination of the microRNA-21. In this work, the two-dimensional MoSe 2 /MXene nanocomposite with high electronic conductivity was synthesized as electrode signal amplification materials to immobilize more capture DNA and accelerate electron transport. After adding microRNA-21, the tripedal DNAzyme walker was activated on the surface of the Pt@CeO 2 nanoclusters, which were as nanozyme to construct the high-performance nanoprobe machine. Then, the tripedal DNAzyme strands could cleave the substrate strands and walk onto the nanoprobe for amplifying the signal remarkably. Furthermore, the detectability of the electrochemical biosensor was verified by DPV, acquiring a wide linear response in a range of 0.1 fM to 1 nM, as well as the limit of detection was 0.04 fM. Hence, such double signal amplified strategy could not only provide excellent selectivity and specificity, but also achieve superior repeatability and stability in real complex serum samples. Therefore, the designed biosensing platform detected different microRNA through modulating the recognition sequence, which might provide a general strategy for various cancer analyses and have a promising potential for clinical application.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2024
·
IF 4.2
Xiaoqin Liu,Jianbo Liu,Wei Li,Qingqing Sheng,Yeming He,Yangyang Wang
Sol–gel method is a low-cost material preparation method; however, it is difficult to obtain a stable sol containing easily hydrolyzable metal ions via this method. In this study, a stable hafnium(IV) oxide (HfO 2 ) sol was prepared by adding benzoyl acetone (BzAcH) modifier. Infrared absorption spectroscopy results showed that the BzAcH additive chelated with the Hf 4+ ions in the sol, thus improving the hydrolysis resistance of the HfO 2 sol, which in turn improved its stability. It was also found that the BzAcH-modified HfO 2 gel film exhibited ultraviolet (UV) photosensitivity. After UV exposure, the film did not dissolve easily in organic solvents . Based on these properties, the micro processing of the HfO 2 film was preliminarily explored, and HfO 2 microstructures were successfully obtained. Additionally, the relative permittivity ( ε r ) of HfO 2 exhibited minimum (∼10.9) and maximum (∼20.6) values at heat-treatment (HT) temperatures of 350 and 450 °C, respectively. With the continuous increase in the HT temperature, ε r first decreased and then increased slightly. Moreover, the current–voltage curves showed that the Pt/HfO 2 /LaNiO 3 (LNO) structure exhibited a pronounced bipolar resistive switching (RS) effect, which was attributed to the fact that LNO could be used as an electrode and an oxygen vacancy (OV 2+ ) storage layer for RS materials. Notably, the oxygen ions in HfO 2 with a low degree of crystallinity are more likely to migrate within its body (which makes it easier to form OV 2+ s), therefore, the “Set” voltage of low-crystallinity HfO 2 films is lower than that of high-crystallinity HfO 2 films. The RS mechanism can be explained by the OV 2+ conductive filament model. These results are of great practical significance for the low-cost preparation of HfO 2 and the application of LNO as an oxide electrode.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2024
·
IF 4.1
An-ru Yan,Xiao-bo Wang,Ling Zhu,Xue-sheng Liu,Zhi-yong Wang
Economic viability and durability are pivotal challenges limiting the commercial application of proton exchange membrane fuel cells (PEMFC). The development of low Pt usage oxygen reduction reaction catalysts with high catalytic activity and durability is imperative. Carbon support corrosion, as well as Pt particles agglomeration and exfoliation are primary causes of commercial Pt/C catalyst degradation. Here, a composite materials formed by TiO 2 containing oxygen vacancy (O V ) and carbon nanotube (CNT) was used as a functional support to successfully load Pt nanoparticles (NPs). The oxygen vacancy facilitated interactions between TiO 2 (O V ) and Pt, enhancing the anchoring of Pt NPs and suppressing particle growth. The Pt/TiO 2 (O V )-CNT demonstrates excellent performance with mass activity of 788 mA/mg Pt @0.85 V, the half-wave potential increased 34 mV and the tafel slope decreased by 11.89 mVdec −1 compared to commercial Pt/C. The durability of Pt/TiO 2 (O V )-CNT nearly 3-fold that of commercial Pt/C with negligible decay of half-wave potential (0.9 %) and mass activity (16 %). Density functional theory calculations and X-ray photoelectron spectroscopy indicated that the charge transfer from TiO 2 (O V ) to Pt facilitates the formation of strong metal-support interactions (SMSI), leading to a downward shift in the d-band center of Pt and a reduction in the binding strength to *OOH, thus lowering the activation energy of the rate-determining step which in turn promoting the activity of ORR. This study provides a reliable approach for designing catalysts with high activity and durability.
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ACS Sensors
·
2024
·
IF 8.2
Hongchao Zhao,Jing Li,Xiaopeng She,Yi Chen,Mengqing Wang,Yanjie Wang,Aijun Du,Cheng Tang,Cheng Zou,Yong Zhou
Sensitive and selective acetone detection is of great significance in the fields of environmental protection, industrial production, and individual health monitoring from exhaled breath. To achieve this goal, bimetallic Au@Pt core–shell nanospheres (BNSs) functionalized-electrospun ZnFe2O4 nanofibers (ZFO NFs) are prepared in this work. Compared to pure NFs-650 analogue, the ZFO NFs/BNSs-2 sensor exhibits a stronger mean response (3.32 vs 1.84), quicker response/recovery speeds (33 s/28 s vs 54 s/42 s), and lower operating temperature (188 vs 273 °C) toward 0.5 ppm acetone. Note that an experimental detection limit of 30 ppb is achieved, which ranks among the best cases reported thus far. Besides the demonstrated excellent repeatability, humidity-enhanced response, and long-term stability, the selectivity toward acetone is remarkably improved after BNSs functionalization. Through material characterizations and DFT calculations, all these improvements could be attributed to the boosted oxygen vacancies and abundant Schottky junctions between ZFO NFs and BNSs, and the synergistic catalytic effect of BNSs. This work offers an alternative strategy to realize selective subppm acetone under high-humidity conditions catering for the future requirements of noninvasive breath diabetes diagnosis in the field of individual healthcare.
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ACS Catalysis
·
2025
·
IF 13.1
Lecheng Liang,Hengyu Li,Peng Li,Jinhui Liang,Shao Ye,Binwen Zeng,Mingjia Lu,Yanhong Xie,Yucheng Wang,Taisuke Ozaki,Shengli Chen,Zhiming Cui
A long-standing puzzle for methanol electrooxidation is the fundamental understanding of the origin of electrocatalytic selectivity. Herein, we unequivocally demonstrate that the Bi-modified Pt/C follows a CO-free dominated pathway during alkaline methanol electrooxidation and unveil the formaldehyde (HCHO) intermediate as a critical factor influencing pathway selectivity. These findings are substantiated by kinetic isotope effects, formate Faradaic efficiency, in situ spectroscopy, ab initio molecular dynamics simulations, and density functional theory calculations. Bi modification significantly increases the HCHO dehydrogenation barrier, which facilitates its desorption and subsequent conversion to the H2COOH– anion at the alkaline interface, intrinsically avoiding CO formation. More specifically, the formation of ensemble sites featuring a V-shaped Bi–Pt–Bi configuration inhibits the cleavage of the C–H bond, and the weak OH binding energy at Bi adatoms effectively prevents blockage of oxygenated species, allowing such ensemble sites to fulfill their functional role. This work provides in-depth insights into the origins of pathway selectivity and benefits the theory-guided design of advanced CO-free electrocatalysts.
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