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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Bifunctional Pd@RhPd Core–Shell Nanodendrites for Methanol Electrolysis

Yu-Chuan Jiang,Hui-Ying Sun,Ya-Nan Li,Jia-Wei He,Qi Xue,Xinlong Tian,Fu-min Li,Shi-Bin Yin,Dong-Sheng Li,Yu Chen

Methanol electrolysis is a promising strategy to achieve energy-saving and efficient electrochemical hydrogen (H2) production. In this system, the advanced electrocatalysts with high catalytic performance for both the methanol oxidation reaction (MOR) and hydrogen evolution reaction (HER) are highly desirable. Inspired by the complementary catalytic properties of rhodium (Rh) and palladium (Pd) for MOR and HER, herein, several Pd core–RhPd alloy shell nanodendrites (Pd@RhPd NDs) are synthesized through the galvanic replacement reaction between Pd nanodendrites (Pd NDs) and rhodium trichloride. For MOR, Pd@RhPd NDs exhibit Rh content-determined catalytic activity, in which Pd@Rh0.07Pd NDs have an optimal combination of oxidation potential and oxidation current due to the synergistic catalytic process of Pd/Rh double active sites. For HER, the introduction of Rh greatly improves the catalytic activity of Pd@RhPd NDs compared to that of Pd NDs, suggesting that Rh is the main activity site for HER. Unlike MOR, however, the HER activity of Pd@RhPd NDs is not sensitive to the Rh content. Using Pd@Rh0.07Pd NDs as robust bifunctional electrocatalysts, the as-constructed two-electrode methanol electrolysis cell shows a much lower voltage (0.813 V) than that of water electrolysis (1.672 V) to achieve electrochemical H2 production at 10 mA cm–2, demonstrating the application prospect of methanol electrolysis for H2 production.

研究领域: 材料科学 · 电化学 · 能源科学
✓ 已验证 DOI 高影响因子
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APPLIED CLAY SCIENCE · 2022 · IF 5.907

Roles of hydrogen bond and ion bridge in adsorption of two bisphenols onto montmorillonite: an experimental and DFT study

Fayang Guo,Dabao Li,Jeremy B. Fein,Jingcheng Xu,Yingwei Wang,Qiaoyun Huang,Xingmin Rong

Reactions occurring at silicate minerals play a significant role in controlling phenolic endocrine disrupting chemicals' bioavailability and mobility. However, the underlying molecular mechanisms for BPA (bisphenol A) and BPS (bisphenol S) onto montmorillonite (MMT) remain poorly understood. To decipher the molecular-level interfacial configuration and dominant reaction mechanism, batch experiments, X-ray diffraction (XRD), Fourier transform infrared spectrum (FTIR), X-ray photoelectron spectroscopy (XPS) measurements, and density functional theory (DFT) calculations were performed. Our batch adsorption experiments showed that MMT exhibits a higher adsorption capacity for BPS than for BPA. The XRD analysis also suggested that BPA and BPS could enter the interlayer of MMT. FTIR and XPS results revealed that The Ca atoms and the oxygen atoms in the SiO 4 tetrahedra were involved in BPA and BPS adsorption process via non-covalent interactions. The electrostatic potential calculations suggested that the sulfonyl O site and the hydroxyl H site on the BPS molecule are more favorable for interacting with the MMT surface than the hydroxyl O and H sites of the BPA molecule. DFT calculations further confirmed that stronger binding of BPS than BPA onto the (001) surface and the interlayer of MMT. BPA tends to form Ca ion bridges through hydroxyl groups onto MMT. In contrast, BPS prefers to form Ca ion bridges onto MMT through its sulfonyl group and form hydrogen bonds via hydroxyl groups. This study provides new insights into the molecular-scale interactions that control BPA and BPS adsorption onto an important and environmentally-relevant clay mineral, and which affect the fate and behavior of BPA and BPS in soil systems.

研究领域: 环境科学 · 分子生物学
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JOURNAL OF MATERIALS SCIENCE · 2022 ·Vol. 57 ·期 27 ·12836-12847 · IF 4.682

Copper containing 3D polyaniline/phytic acid hydrogels for photocatalytic hydrogen production

Pan Xueling,Wu Sheng,Wang Tingting,Histand Gary,Li Yingwei

Abstract A Cu-PP hydrogel with 3D network was synthesized using a simple in-situ polymerization method. PA (phytic acid) acts as the dopants and crosslinking agent to form PANI-PA (polyaniline-phytic acid) hydrogel via in-situ polymerization of aniline. PA is also used as a chelating agent to coordinate with Cu 2+ ion due to the high coordination capacity. When irradiated by light, Cu 2+ was slowly reduced to form Cu NPs, distributing uniformly in the 3D matrix of PANI-PA. The 3D network nanostructure ensures a complete contact between the photocatalyst and water, promoting the separation of electrons and holes. The introduction of PANI-PA improves the separation efficiency of electron-hole pairs, where PANI-PA acts as a hole reservoir to trap the holes generated by Cu NPs, hindering the recombination of electron-hole pairs. The Cu 0.2 -PP hydrogel with a copper content of 30.8% exhibits the best hydrogen production rate (6.09 mmol·g −1 ·h −1 ), which is 6.7 times greater than that of pure Cu NPs. Graphical abstract

研究领域: 材料科学 · 能源科学
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Food Biophysics · 2020 ·Vol. 15 ·期 4 ·452-462 · IF 2.387

Structure and Properties of Organogels Developed by Diosgenin in Canola Oil

Zeng Chaoxi,Wan Zheng,Xia Huiping,Zhao Haiyang,Guo Shiyin

In this study, naturally occurring ingredient diosgenin was utilized as an organogelator for structuring canola oil. Results show that stable diosgenin-based organogel can be obtained at only 2% of diosgenin concentration when the gel preparation temperature is 100 °C. Oil binding capacity and rheological properties of the organogel were investigated. Results demonstrate that these two macroscopic characteristics of the organogels can be significantly modified by simply changing the gel preparation temperature or diosgenin concentration. When the preparation temperature was 120 °C and the diosgenin concentration higher than 4%, oil binding capacity of at least 90% were obtained. Furthermore, higher gel preparation temperature resulted in higher G′values of the diosgenin-based organogels. According to the results analyzed by polarized light microscopy, XRD and FT-IR, it can be found that the possible gelation mechanism of the diosgenin-based organogels is formation of supramolecular structures by self-assembly of diosgenin molecule crystals via hydrogen bonding interaction. Varying gel preparation conditions of the organogels lead to self-assembly of diosgenin molecules to form different microstructures. Therefore, diosgenin can be considered as a good organogelator for producing functional organogel from canola oil. The novel diosgenin-based organogel is expected to be widely used in bio-related fields such as food and pharmaceutical industries.

研究领域: 食品科学 · 材料科学
✓ 已验证 DOI 高影响因子
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2021 · IF 3.171

Nb2O5 promoted Pd/AC catalyst for selective phenol hydrogenation to cyclohexanone

Chunhua Zhang,Zhengyan Qu,Hong Jiang,Rizhi Chen,Weihong Xing

Phenol hydrogenation is a green route to prepare cyclohexanone, an intermediate for the production of nylon 66 and nylon 6. The development of high-performance catalysts still keeps a great challenge. Herein, the activated carbon (AC) was modified with an acidic material Nb 2 O 5 to adjust the microstructure and surface properties of AC, and the influences of the calcination temperature and Nb 2 O 5 content on the catalytic performance of the Pd/AC-Nb 2 O 5 catalysts for the phenol hydrogenation to cyclohexanone were investigated. The Nb 2 O 5 with proper content can be highly uniformly distributed on the AC surface, enhancing the acidity of the Pd/AC-Nb 2 O 5 catalysts with comparable specific surface area and Pd dispersion, thereby improving the catalytic activity. The hybrid Pd/AC-10Nb 2 O 5 -500 catalyst exhibits the synergistic effect between the Pd nanoparticles and AC-10Nb 2 O 5 , which enhances the catalytic activity for the hydrogenation of phenol. Furthermore, the as-prepared Pd/AC-10Nb 2 O 5 -500 catalyst shows good reusability during 7 reaction cycles.

研究领域: 化学工程 · 催化材料
✓ 已验证 DOI 高影响因子
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OPTICAL MATERIALS · 2022 · IF 3.754

Photocatalytic H2 evolution properties of K0.5Na0.5NbO3 (KNN) with halloysite nanotubes

Jian Lu,Hui Lin,Ruijin Hong,Dawei Zhang

By the solid phase reaction method, pure KNN and KNN with different proportions halloysite nanotubes (HNTs) were prepared to study the photocatalytic hydrogen evolution performance under the UV light irradiation. The band gaps of KNN with HNTs are narrower than that of pure KNN. The absorbance of KNN in the ultraviolet region is significantly enhanced by the incorporation of HNTs, where the absorbance in the 200-300 nm region increased about 2 times. Compared with KNN, the conduction band edge of KNN-5wt%HNTs reduced from −1.13 eV to −1.18 eV, showing stronger reducing ability. The H 2 production rate of KNN with HNTs is much higher than that of the raw KNN without HNTs. The best H 2 production rate of KNN-5wt%HNTs is 31.28 μmol•g −1 •h −1 , approximate 4.48 times as high as the rate of pure KNN (6.98 μmol•g −1 •h −1 ), suggesting appropriate addition of HNTs can efficiently improve the H 2 production efficiency.

研究领域: 材料科学 · 能源科学
✓ 已验证 DOI 高影响因子
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FUEL · 2019 · IF 5.128

Study on competitive absorption of SO3 and SO2 by calcium hydroxide

Kejia He,Qiang Song,Zhennan Yan,Na Zheng,Qiang Yao

Alkaline injection is an effective way to control the emission of high concentration SO 3 caused by the use of high-sulfur coal and selective catalytic reduction (SCR), but its performance is affected by the competitive absorption of SO 2 . A fixed-bed reactor was used to study the competitive absorption of SO 3 and SO 2 by Ca(OH) 2 . The dynamic absorption curves in different atmospheres were obtained, the intermediate products were characterized, and the competitive absorption mechanism was discussed. The absorption of SO 3 and SO 2 consists of the chemical kinetics-controlled and product layer diffusion-controlled stages. In the chemical kinetics-controlled stage, the SO 3 and SO 2 removal efficiencies were around 90% and 55% at first and then decreased; the SO 3 selectivity was around 0.1 at first and then increased. In the product layer diffusion-controlled stage, the SO 3 removal efficiency gradually decreased but kept greater than 10%, while the SO 2 removal efficiency deceased to zero; the SO 3 selectivity continued to increase and reached 0.31 at most when SO 2 absorption ceased. There existed significant competition between SO 3 and SO 2 absorption. The increasing SO 3 concentration promoted the SO 3 absorption and the increasing SO 2 concentration decreased it. The absorption of SO 3 increased the intensity of the SO 4 2 - SO42- band, decrease the intensity of the SO 3 2 - SO32- band, and made the product layer more compact. The possibility of SO 3 reacting with the components (CaSO 3 , CaSO 4 and CaCO 3 ) on the reacted Ca(OH) 2 surface was analyzed. Ionic diffusion was proposed as the main mechanism of the continuous SO 3 absorption after the formation of a dense product layer.

研究领域: 环境科学 · 化学工程
✓ 已验证 DOI 高影响因子
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Carbon dots-Pt modified polyaniline nanosheet grown on carbon cloth as stable and high-efficient electrocatalyst for hydrogen evolution in pH-universal electrolyte

Qian Dang,Yuyang Sun,Xiao Wang,Wenxiang Zhu,Ying Chen,Fan Liao,Hui Huang,Mingwang Shao

Design and fabrication of hydrogen evolution reaction (HER) electrocatalysts with high activity, durability and moderate price are vital for realizing a viable water-splitting technology. Here, we demonstrate the carbon dots-Pt modified polyaniline nanosheets grown on carbon cloth (CDs/Pt-PANI) can serve as stable and high-efficient electrocatalyst in pH-universal electrolyte for HER. The overpotential for optimal CDs/Pt-PANI electrocatalyst can be lowered to 30 mV at 10 mA·cm −2 when Pt loading was only 8.1 μg·cm −2 (the Pt content in commercial 20 wt% Pt/C is 22.4 μg·cm −2 ), showing exceptional HER efficiency with a small Tafel slope 41.7 mV·dec −1 in acidic solution. Meanwhile, the optimal CDs/Pt-PANI electrocatalyst exhibits well stability with 17 mV potential shift after 20 h, which is 0.06 times than that of commercial 20 wt% Pt/C (286 mV). It is noticeable, the optimal CDs/Pt-PANI electrocatalyst is superior to 20 wt% Pt/C with HER performance in pH-universal electrolyte (acidic, neutral and basic). The efficient and stable HER performance of CDs/Pt-PANI should ascribe to the synergy in the CDs, Pt and PANI, in which the surface functional groups of CDs can connect tightly with PANI and improve the stability of Pt, simultaneously, the PANI and Pt provide the high-efficiency in HER.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

N, O-Doped surface modulation of ZnIn2S4 with high hydrophilicity for enhanced photocatalytic hydrogen evolution

Tingyuan Zhang,Lingxiao Song,Jiahui Yang,Jiajia Wang,Dong Feng,Baojun Ma

Heteroatom doping is a promising strategy for optimizing the photocatalytic activity of semiconductors. However, relying solely on single-element doping often poses challenges in modulating the capabilities of semiconductors. Herein, we adopt a strategy of simultaneously modifying ZnIn 2 S 4 with the double non-metallic elements nitrogen (N) and oxygen (O) to form (N, O)-ZnIn 2 S 4 . Interestingly, (N, O)-ZnIn 2 S 4 exhibits significantly higher hydrophilicity and specific surface area compared to pristine ZnIn 2 S 4 . The contact angle decreases from 24° to 21°, while the specific surface area increases from 56 m 2 /g to 75 m 2 /g. The hydrogen production rate of (N, O)-ZnIn 2 S 4 reaches 400 μmol/h/g, which is 2.52 times higher than that of pristine ZnIn 2 S 4 . Photoelectrochemical characterization reveals that (N, O)-ZnIn 2 S 4 has a lower overpotential, higher photocurrent, lower resistance, reduced fluorescence intensity, and shorter fluorescence lifetime. Additionally, co-catalyst loading boosts the hydrogen production activity of ZnCo 2 S 4 /(N, O)-ZnIn 2 S 4 from 548 μmol/h/g to 810 μmol/h/g, compared to ZnCo 2 S 4 /ZnIn 2 S 4 . This study presents a dual non-metallic modification strategy to enhance semiconductor properties, achieving superior performance in photocatalytic hydrogen production.

研究领域: 材料科学 · 能源科学
✓ 已验证 DOI PubMed 高影响因子
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Functional Materials Letters · 2024 · IF 1.2

Ruthenium-doped Ni5P4 for hydrogen production via water electrolysis

Yaoting Wang,Zhiling Chou,Huimin Zhang,Yiming Zou,Junfu Wang,Haochen Ding,Hong Zhao,Song Wang,Xin Xiao

The electrochemical decomposition of water to produce hydrogen using clean energy sources has become a sustainable pathway for hydrogen utilization, with efficient hydrogen evolution reaction (HER) electrocatalysts crucial for high energy conversion efficiency. Nickel phosphide is widely utilized in the electrocatalytic HER owing to its unique electronic properties, efficient electrocatalytic performance, and excellent corrosion resistance. However, the HER activity of nickel–phosphide electrocatalysts remains low, necessitating further research for practical applications. This paper introduces a method for preparing Ru-doped Ni 5 P 4 , including the mechanism of the HER, the preparation of Ru@Ni 5 P 4 , and its performance in electrocatalytic hydrogen evolution. The preparation methods for the Ru@Ni 5 P 4 electrocatalyst were classified, with a focus on the preparation techniques and research progress regarding its HER activity. The HER activities of the pure Ni 5 P 4 , Ru@Ni 5 P 4 , and 10 wt.% Pt/C electrodes were compared based on experimental indicators such as the overpotential and Tafel slope at a specific current density.

研究领域: 材料科学 · 电化学 · 能源化学 · 催化化学 · 可持续能源
✓ 已验证 DOI 高影响因子
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Polymers · 2024 ·Vol. 16 ·期 13 ·1946 · IF 4.7

Experimental Study on the Transport Properties of 12 Novel Deep Eutectic Solvents

Jing Fan,Yuting Pan,Dazhi Gao,Hongwei Qu

Deep eutectic solvents (DESs) are complex substances composed of two or three components, wherein hydrogen bond donors and acceptors engage in intricate interactions within a hydrogen bond network. They have attracted extensive attention from researchers due to their easy synthesis, cost-effectiveness, broad liquid range, good stability, and for being green and non-toxic. However, studies on the physical properties of DESs are still scarce and many theories are not perfect enough, which limits the application of DESs in engineering practice. In this study, twelve DESs were synthesized by using choline chloride and betaine as HBAs, and ethylene glycol, polyethylene glycol 600, o-cresol, glycerol, and lactic acid as HBDs. The variation rules of their thermal conductivity and viscosity with temperature at atmospheric pressure were systematically investigated. The experimental results showed that the thermal conductivity of the 1:4 choline chloride/glycerol solvent was the largest at 294 K, reaching 0.2456 W·m−1·K−1, which could satisfy the demand for high efficiency heat transfer by heat-transferring workpieces. The temperature–viscosity relationship of the DESs was fitted using the Arrhenius model, and the maximum average absolute deviation was 6.77%.

研究领域: 化学工程 · 材料科学
✓ 已验证 DOI PubMed 高影响因子
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FUEL · 2021 · IF 6.609

Hydrogen-rich syngas production from chemical looping gasification of lignite by using NiFe2O4 and CuFe2O4 as oxygen carriers

Kun Zhao,Xiaojie Fang,Zhen Huang,Guoqiang Wei,Anqing Zheng,Zengli Zhao

Chemical looping gasification provides a novel technology to enable clean conversion of coal with inherent CO 2 capture. In this study, four types of NiFe 2 O 4 and CuFe 2 O 4 synthesized by sol–gel method and solid-phase method were used as oxygen carriers to promote the H 2 production from gasification of lignite. The effects of the types of oxygen carrier and oxygen carrier to coal (O/C) ratio on chemical looping gasification of lignite were first investigated by a thermogravimetric analyzer (TGA) combing with various analytical methods. The results show that, among four types of oxygen carrier, the NiFe 2 O 4 synthesized by sol–gel method exhibits the highest gasification reactivity with lignite char at an O/C ratio of 1, since its highly cubic spinel structure is beneficial to improve the mobility of lattice oxygen. Furthermore, the operating conditions for chemical looping gasification of lignite were optimized and the gasification performance of four types oxygen carriers was compared by using a fixed bed reactor. It is found that NiFe 2 O 4 synthesized by sol–gel method exhibits the highest total gas yield of 24.47 mol/kg and H 2 /CO ratio of 0.77 during chemical looping gasification of lignite under the optimal operating conditions, ascribed to Fe-Ni synergistic effect which provided higher gasification reactivity with lignite char. The addition of steam drastically improves the total gas yield and H 2 /CO ratio of syngas from 24.47 mol/kg and 0.77 to 64.98 mol/kg and 2.79, suggesting that the H 2 /CO ratio of syngas can be flexibly adjusted to meet the need of downstream process via controlling the amount of steam added. These findings provide an efficient method to obtain H 2 -rich syngas via chemical looping gasification of lignite.

研究领域: 能源科学 · 材料科学
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