ACS Applied Materials & Interfaces
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2023
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IF 9.5
Jin Wang,Zhongyan Gong,Yulong Zhang,Yaxin Song,Xinya Chen,Zhihao Lu,Lu Jiang,Chengcheng Zhu,Kun Gao,Kaili Wang,Junjie Wang,Liuyingzi Yu,Soukaina Khayour,Haijiao Xie,Zhuoyao Li,Gang Lu
Electrocatalytic hydrogen evolution reaction (HER) is receiving increasing attention as an effective process to produce clean energy. The commonly used precious metal catalysts can be hybridized with semiconductors to form heterostructures for the improvement of catalytic efficiency and reduction of cost. It will be promising to further improve the efficiency of heterostructure-based nanocatalysts in electrocatalytic and photocatalytic HER using a simple and effective method. Herein, we improve the efficiency of Au/TiO2 in electrocatalytic and photo-electrocatalytic HER by selectively adsorbing p-aminothiophenol (PATP) molecules. The PATP molecules are adsorbed on the gold surface by using a simple solution-based method and favor the charge separation at the Au–TiO2 interface. We also compare the PATP molecules with other thiophenol molecules in the enhancement of electrocatalytic HER. The PATP-induced enhancement in electrocatalysis is then further investigated by density functional theory (DFT) calculations, and this enhancement is attributed to a reduction in Gibbs energy of adsorbed hydrogen after surface adsorption of PATP molecules. This work provides a simple, cost-effective, and highly efficient approach to improve the electrocatalytic and photo-electrocatalytic efficiency of Au/TiO2, and this approach could be easily extended to other heterostructure-based nanocatalysts for performance enhancement and may be used in many other catalytic reactions.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Xinsheng Tang,Tursun Abdiryim,Ruxangul Jamal,Xiong Liu,Fangfei Liu,Feng Xu,Abdukeyum Abdurexit,Qian Cheng,Nawrzhan Serkjan,Shuyue Xie,Yiming Liu
TiO 2 -based ultraviolet (UV) photodetectors (PDs) with broadband optical detection range are widely used in commercial and military applications. Nevertheless, the self-powered UV PDs of TiO 2 nanoarrays (NRs) have relatively low response rates and slow response times. Here, a high responsivity self-powered p-n heterojunction UV PD based on TiO 2 NRs: CQDs/FTO and PEDOS/FTO is fabricated by a simple face-to-face assembly process. The pyroelectric effect of TiO 2 NRs is enhanced by sensitizing TiO 2 NRs with CQDs, which would reduce the bandgap value of TiO 2 NR, broaden the range of photoresponse, and reduce recombination of electron-hole. Furthermore, the pyro-phototronic effect of CQDs, the energy level matching from CQDs to PEDOS and the interaction between –OH in CQDs and ethylene oxide groups in PEDOS enhance the performance of the prepared UV PDs. The TiO 2 NRs: CQDs//PEDOS UV PDs achieve a high photo-responsivity and photo-detectivity of 150.95 mA/W and 3.73 × 10 11 Jones at 0 bias (365 nm), respectively, which are better than those at wavelengths of 380 nm. We also found that the photocurrent induced via the pyro-phototronic effect increases with the light power intensity. This work points the way for photovoltaic and photo-induced pyro-phototronic effects to improve the performance of TiO 2 NRs-based UV PDs.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Lei Chen,Jiankun Zhang,Qingxue Li,Yangyang Zhang,Jiajia Huangpu,Jiaqi Shen,Mingye Gu,Jiaxiang Yang
Straw biochar loaded zero-valent iron nanoparticles were prepared by co-precipitation method using agricultural waste straw biochar as a carrier for the removal of p-nitrophenol (PNP) by activated sodium persulfate (PS). The physicochemical properties of BC@nZVI were characterized using SEM, EDS, FTIR, BET, and RAMAN. The effects of PS concentration, catalyst concentration, initial pH, coexisting anions, and different activation systems on the degradation of PNP were investigated. The results showed that the best activation effect was exhibited at pH= 7, BC@nZVI dosage of 2 g/L, and PS concentration of 1 mM, and the removal of 40 mg/L PNP reached 91.7 % in 10 min. The high concentration of PS (4 mM) triggered free radical competition to inhibit the degradation, and the removal rate was only 74.5 % at 1 mM. In addition, bicarbonate ions (0–20 M) had a significant inhibitory effect on this system. Electron spin resonance (ESR) demonstrated that SO 4 ⋅ − and·OH were the major radicals, and SO 4 ⋅ − was preferentially generated. The intermediate products were identified by LC-MS, XRD and XPS characterization, which showed that adsorption and redox were the main degradation mechanisms, with p-benzoquinone was the oxidized product and substances such as 4-heptanone and propionic acid were the reduced products. This study proves that BC@nZVI activated PS is an efficient and excellent means of removing PNP and a good way to reuse agricultural waste.
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Journal of the Taiwan Institute of Chemical Engineers
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2023
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IF 5.7
Zhixin Chen,Boyuan Ning,Yanqing Cai,Minghua Liu,Pingfan Xu,Peikun Zhang,Guangcan Xiao,Yunhui He
Background The accumulation of antibiotics in water systems has received considerable global attention due to its detrimental effects. There is an urgent need to develop rapid and efficient methods for the degradation of antibiotics. Methods In this work, a highly efficient AgFeO 2 /Ag 3 VO 4 photocatalyst was successfully fabricated by a hydrothermal method and analyzed using different techniques. Under visible light irradiation, photocatalytic behavior of AgFeO 2 /Ag 3 VO 4 heterojunctions in the degradation of levofloxacin is investigated. Significant findings The results showed that p-n heterojunction was formed between AgFeO 2 and Ag 3 VO 4 , which improved the separation and transfer of photogenerated charge carrier under the action of the internal electric field. The apparent reaction rate of AgFeO 2 /Ag 3 VO 4 heterostructure toward degradation of levofloxacin reached to 0.2770 min −1 , which was about 2.15 times and 36.73 times larger than those of Ag 3 VO 4 and AgFeO 2 , respectively, and much larger than other counterparts. Furthermore, possible photocatalytic degradation pathway of levofloxacin was comprehensively determined by LC-MS analysis. This work would provide in-depth understanding on the efficient photocatalytic removal of antibiotics for sustainable environmental remediation.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2023
·Vol. 170
·期 9
·096501
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IF 3.9
Kangli Chen,Yuan Li,Guanjiu Wu,Qing Wang,Chenfeng Fan,Lu Zhang,Jianzheng Song,Shumin Han
Designing Earth-abundant, cost-effective catalysts for hydrogen evolution via water splitting is essential for hydrogen generation. Adding a third metal element to binary phosphides provides the opportunity to tune their morphology, crystalline and electronic structures and thus their electrocatalytic properties. In this study, a hierarchical crystalline/amorphous Ni−Co−P compound is prepared on nickel foam (NF) with different nickel to cobalt ratio by one-step electrodepositing technique. The Ni−Co−P/NF is composed of metallic Co and amorphous phosphides. It has hierarchical morphology, consisting of ∼800 nm spherical particles in the bottom layer, ∼1.5 μm spherical particles in the middle layer, and staggered network structure on the top layer. The Ni−Co−P/NF electrode exhibits superior hydrogen evolution reaction (HER) catalytic activity in the alkaline solution, which requires only 72 mV for delivering 10 mA cm−2. More importantly, the Ni−Co−P/NF catalyst sustains the current density of 20 mAcm−2 for 53 h with negligible degradation in overpotential which shows remarkable electrochemical stability.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Li Li,Kaixuan Kuang,Xiuzhen Zheng,Jiahui Wang,Wei Ren,Jingbiao Ge,Sujuan Zhang,Shifu Chen
To enhance the efficiency of photocatalytic H 2 evolution, numerous methods are employed by increasing the utilization of photogenerated charge carriers (PCCs), including catalyst design, defect regulation, and selection of suitable H + resources. Using self-assembly method, CoWO 4 /Zn x Cd 1−x S with p–n heterojunction was synthesized. Although CoWO 4 (CW) cannot produce H 2 under visible light irradiation, it can provide photogenerated electrons (e − ) to Zn 0.3 Cd 0.7 S (ZCS), and largely increase the photocatalytic activity of ZCS. The optimal CW/ZCS composite can reach 15.58 mmol·g −1 ·h −1 , which is 45.8 and 24.3 times higher than the values of the pure CdS and ZCS, respectively. The largely enhanced photocatalytic H 2 production is attributed to the Zn vacancies (V Zn ), p–n heterojunction, and p-chlorobenzyl alcohol (Cl–PhCH 2 OH) as the H + source of H 2 production. V Zn on the ZCS surface as the capture center of photogenerated holes (h + ), can regulate the carrier distribution, which results in more photogenerated e − and less generated h + . The combination of p–n heterojunction and V Zn can enhance the separation and transfer efficiency of PCCs, and effectively inhibit the recombination of charge carriers. To further improve the utilization rate of PCCs, the photocatalytic H 2 evolution is proceeded by Cl–PhCH 2 OH oxidation in N , N -dimethylformamide solution, with 4-chlorobenzaldehyde (Cl–PhCHO) generated. The separated photogenerated e − and h + both participated in the redox reaction of H + reduction and Cl–PhCH 2 OH oxidation, considering that the amount of H 2 and Cl–PhCHO products are close to 1:1. This work not only facilitates the separation and transfer of PCCs, but also provides directions for the design of efficient photocatalysts and H 2 evolution in the organic phase.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
·
IF 8.4
Changlin Xiao,Zihuan Tang,Zhuangzhuang Ma,Xiaotong Gao,Hongqiang Wang,Lichao Jia
Metal oxides based semiconductors promise high performance gas sensing owing to their robustness and low cost, but are limited by their unsatisfied adsorption ability and intrinsic low carriers' mobility. We herein demonstrate an efficient strategy of reducing the adsorption energy and improving the carrier mobility via bulk implanted TiO 2 nanocrystals (NCs) in LaFeO 3 porous structure . By implanting laser generated sub-3 nm TiO 2 NCs in LaFeO 3 samples, the response value (221.8 for 100 ppm formaldehyde) increases about 4 times comparing with that of pristine. Additionally, the sample exhibits high sensitivity and fast response/recovery speed toward formaldehyde steam. The detailed analyses and theoretical calculation proves that the TiO 2 NCs could cause the increase of adsorbed oxygen levels as well as the carrier mobility through forming the heterojunction with LaFeO 3 . This work verifies that TiO 2 NCs implanted LaFeO 3 is a promising formaldehyde sensing material, which provides a new approach to improve sensing ability of metal oxide semiconductor (MOS) based gas sensors.
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Journal of Materials Research and Technology-JMR&T
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2023
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IF 6.4
Shan Zhang,Yupeng Lu,Yahao Geng,Yixin Yin,Guiyong Xiao
Hydroxyapatite (HA) is an important component of mammalian bones and teeth. Its superior biocompatibility, biological activity, and bone tissue regenerative properties make it an ideal material for bone tissue replacement and regeneration. The morphological characteristics of HA can affect its selection in various applications. In contrast, one-dimensional (1D) micro/nano-structured HA has received widespread attention in the field of biomedicine. In particular, HA ultra-long nanofibers possess excellent mechanical properties, such as flexibility and deformability, overcoming the brittleness of traditional HA ceramic materials. This work successfully synthesized HA ultra-long nanofibers using oleic acid as a template by a solvothermal method. Particularly, the effects of the initial Ca/P ratios (iCa/P) on the morphologies of HA products were investigated. The microstructure and properties of HA products were characterized by scanning electron microscopy (SEM), X-ray powder diffractometer (XRD) and Fourier transform infrared spectroscopy (FTIR). The results indicated that the uniform and flexible HA nanofibers can be obtained only under the appropriate iCa/P. In addition, the effect of iCa/P on the microstructures of the HA formation stages was investigated using transmission electron microscopy (TEM), and then the formation mechanism of HA nanofibers was proposed. In this process, it is found that HA nanofibers mainly grow selectively along the c-axis, while iCa/P precisely influences the preferential growth direction of HA products.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Weirui Chen,Siyou Fu,Xukai Li,Jing Wang,Xunan Ning,Liying Bin,Ping Li,Bing Tang,Laisheng Li
Photocatalytic ozonation (PCO) was a novel water treatment method, but the low photo-generated electron ( e - ) utilization and ambiguous ROS formation mechanism restrained its performance. Herein, C vacancy and F co-decorated g-C 3 N 4 (FCN_Cv) was designed to accelerate the PCO performance with sodium p -perfluorinated nonoxybenzenesulfonate (OBS) acting as model pollutant. Comparative characterizations revealed that FCN_Cv remained the inherent structure of g-C 3 N 4 (BCN), and had an enhanced conduction band potential, narrower band gap and longer e - lifetime. FCN_Cv exhibited the greater activity over BCN, with 99.3 % OBS removal in 30 min but only 78.3 % for BCN during PCO process. •OH was the main ROS for degrading OBS. The greater •OH yield was obtained by FCN_Cv PCO process because of the increase of e - utilization. On one hand, the two electrons reduction of O 2 into H 2 O 2 on FCN_Cv was accelerated, which triggered the peroxone reaction between photogenerated-H 2 O 2 and O 3 . On the other hand, the direct one electron reduction of O 3 by e - also accounted for •OH generation. 17 kinds of intermediates were detected and the OBS degradation routes were inferred, which was involved with hydroxylation, C-O cleavage and aromatic ring opening reactions. Overall, this study demonstrated the feasibility of decorating F element and C vacancy on g-C 3 N 4 in enhancing e - utilization and •OH generation during PCO process as well as deepened the understanding of fate of OBS in PCO process.
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GREEN CHEMISTRY
·
2023
·Vol. 26
·期 2
·968-978
·
IF 9.8
Xinwei Wen,Yue Zhao,Puyang Fan,Jiajie Wu,Kai Xiong,Chang Liu,Qing Qu,Lei Li
The production of ammonia under ambient conditions has been a long-standing challenge for the chemical industry. The electroreduction of nitrate presents a promising solution for nitrate wastewater treatment and decentralized ammonia production. However, traditional Ag-based catalysts suffer from nitrate-to-nitrite conversion, leading to toxicity concerns and hampering ammonia preparation. In this study, we synthesized an innovative Ag–Cu–P catalyst that effectively tunes the d-band centre and electronic structure. The catalyst exhibited a remarkable NH4+ yield rate of 566.30 μmol cm−2 h−1 at −0.3 V (vs. RHE), reducing nitrite content to below the drinking water standard. Characterization results revealed a distinctive fern leaf-like morphology, providing an expanded active surface area. The challenge of facile nitrate conversion to nitrite on Ag-based catalysts has been addressed through the implementation of electronic structure modulation in this work. Theoretical calculations confirmed the substantial reduction in the energy barrier by modulating the d-band centre and electronic structure, facilitating the conversion of nitrite to ammonia. The regulation and analysis of d-band centres yielded valuable insights for catalyst material design. Meanwhile, direct evidence for potential intermediates has also been presented through in situ spectroscopy. These findings hold significant potential for practical applications, such as enhanced wastewater treatment and decentralized ammonia production, and provide support in the pressing need for sustainable ammonia synthesis under ambient conditions.
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Surfaces and Interfaces
·
2023
·
IF 6.2
Xinsheng Tang,Hujun Zhang,Ruxangul Jamal,Abdukeyum Abdurexit,Nawrzhan Serkjan,Shuyue Xie,Yiming Liu,Tursun Abdiryim
A self-powered ultraviolet photodetector (UV PD) effectively utilizes UV energy and has attracted greatly attention due to its no consuming of any external power. In this work, TiO 2 nanoarrays (NRs) were synthesized by a one-step hydrothermal method, which was combined with P(TTh-co-EDOT) to realize a high-performance p-n heterojunction UV PD, and P(TTh-co-EDOT) was evaluated as the photosensitive layers in UV PDs for the first time. Furthermore, the working mechanism for the self-powered of UV PD was discussed in detail based on the energy band theory. Different electrochemical deposition cycles of TTh-co-EDOT on the surface of TiO 2 NRs were applied to form p-n heterojunction for achieving the optimum photoelectric performance. Among them, it was found that the optimum UV PD based on face-to-face fabrication of TiO 2 NRs and P(TTh-co-EDOT) from 3 deposition cycles exhibits an enhancement of photoelectric performance without applying any external voltage. Benefiting from the enhanced built-in electric field of the TiO 2 NRs/P(TTh-co-EDOT) interface, balancing photogenerated carriers and the charge separation and transport in self-power mode, the responsivity and detectivity of TiO 2 NRs/P(TTh-co-EDOT)-3C are 2.252 mA/W and 3.413 × 10 10 Jones, with the rise and fall times are 0.256/0.427 s, which exhibited excellent photoelectric properties and stability. TiO 2 NRs/P(TTh-co-EDOT)-1C has the lowest responsivity (0.0995 mA/W) and detectivity (6.035 × 10 9 Jones) and TiO 2 NRs/P(TTh-co-EDOT)-4C has the longest rise and fall times (0.460/0.451 s). These results suggest that the great potential of the TiO 2 NRs and P(TTh-co-EDOT) for high-performance UV PDs.
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EUROPEAN POLYMER JOURNAL
·
2023
·
IF 6
Hao Su,Zhenxiao Zhang,Weixing Song,Kaixiang Shi,Fei Cheng,Meng Hao,Yijia Ma,Yuanbo Chen,Guangfeng Wu,Ying Song
In this study, a novel electrochromic hydrogel AG/P(AAm-AAc)/P 2 W 18 was prepared by loading polyoxometalate K 6 P 2 W 18 ·10H 2 O (P 2 W 18 ) into a double-network hydrogel formed with agar (AG) and copolymer of polyacrylamide (PAAm) and polyacrylic acid (PAAc). The mechanical properties of hydrogels can be tuned by adjusting the proportion of PAAc in the copolymer P(AAm-AAc). Electrochromic hydrogel shows the best mechanical properties when the proportion of PAAc is 10 % (AG/P(AAm-AAc)-10/P 2 W 18 ), and the maximum elongation at break and the fracture stress are about 2.0 and 2.5 times higher than that of pure PAAm. P 2 W 18 gives good electrochromic properties to the hydrogels without the addition of electrolytes. Under the external voltage, the electrochromic hydrogel changes from colorless to blue with the optical contrast up to 65.54 % at 700 nm. The electrochromic device based on this hydrogel is simple in structure, easy to manufacture and highly stretchable, which has good application potential in the field of wearable electronics.
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