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JOURNAL OF MATERIALS SCIENCE · 2017 ·Vol. 52 ·期 13 ·8207-8218 · IF 2.599

Design and fabrication of size-controlled Pt–Au bimetallic alloy nanostructure in carbon nanofibers: a bifunctional material for biosensors and the hydrogen evolution reaction

Zhang Bin,Zhu Han,Zou MeiLing,Liu XinRong,Yang Hui,Zhang Ming,Wu WeiWei,Yao JuMing,Du MingLiang

Small-sized and well-dispersed Pt–Au nanoparticles (Pt–AuNPs) grown on carbon nanofibers (Pt–AuNPs/CNFs) with excellent electroanalytical and electrocatalytic performance in the detection of H 2 O 2 and the catalytic hydrogen evolution reaction (HER) were designed and fabricated via electrospinning technology and an in situ thermal reduction process. Large numbers of Pt–AuNPs were homogenously distributed on the CNFs. A Pt–AuNP/CNF hybrid with low Pt content was utilized as a bifunctional electrocatalyst, exhibiting a higher response current of 116 μA without an enzyme in the detection of H 2 O 2 and a lower overpotential ( j  = 10 mA cm −2 at −235 mV) and Tafel slope (84 mV decade −1 ) for HER than the PtNPs/CNFs and the AuNPs/CNFs. These results were ascribed to the specific nanostructure of the well-dispersed Pt–AuNPs, the favorable electron transport capability, the excellent durability of the CNFs, and the enhanced surface-specific area of the Pt–AuNPs/CNFs. This study offers a green and facile method for constructing a specific bimetallic nanostructure for application in catalytic fields.

研究领域: 材料科学 · 电化学 · 纳米技术 · 催化领域
✓ 已验证 DOI 高影响因子
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JOURNAL OF MOLECULAR LIQUIDS · 2021 · IF 6.165

On-demand hydrogen evolution upon magnetic composite-nanocatalyzed sodium borohydride hydrolysis

Yi Wang,Jialu Shen,Hailin Tian,Xiang Liu,Yingping Huang

Fast and convenient hydrogen evolution under ambient condition from stable hydrogen-rich materials is highly awaited. Herein, a series of magnetic nanocomposites are reported as robust catalysts for promoting H 2 evolution upon hydrolysis of sodium borohydride . The optimized Ni 2 Rh-, Ni 2 Pd- and Ni 2 Pt/Fe 3 O 4 nanocomposites exhibit outstanding catalytic performances on NaBH 4 hydrolysis with remarkable TOF values of 72.2, 69.2 and 46.1 L(H 2 )·g. cat −1 ·min −1 , respectively, due to sharp volcano-type synergetic effect between Ni and the noble metal . Based on the Arrhenius equation, the activation energy ( E a ) of the hydrolysis of NaBH 4 is 54.95 kJ/mol with the catalyst Ni 2 Pt/Fe 3 O 4 . The Ni 2 Pt/Fe 3 O 4 has been successfully recycled 5 times and applied as an efficient “on–off” switch for on-demand H 2 evolution.

研究领域: 化学 · 材料科学 · 能源科学
✓ 已验证 DOI 高影响因子
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CHINESE CHEMICAL LETTERS · 2020 · IF 4.632

Ceria supported Ru0-Ruδ+ clusters as efficient catalyst for arenes hydrogenation

Yanwei Cao,Huan Zheng,Gangli Zhu,Haihong Wu,Lin He

Selective hydrogenation of aromatic amines , especially chemicals such as aniline and bis(4-aminocyclohexyl)methane for non-yellowing polyurethane, is of particular interests due to the extensive applications. To conquer the existing difficulties in selective hydrogenation, the Ru 0 -Ru δ + /CeO 2 catalyst with solid frustrated Lewis pairs was developed for aromatic amines hydrogenation with excellent activity and selectivity under relative milder conditions. The morphology, electronic and chemical properties, especially the Ru 0 -Ru δ + clusters and reducible ceria were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electronic microscopy (SEM), X-ray photoelectron spectroscopy (XPS), CO 2 temperature programmed desorption (CO 2 -TPD), H 2 temperature programmed reduction (H 2 -TPR), H 2 diffuse reflectance Fourier transform infrared spectroscopy (H 2 -DRIFT), Raman, etc . The 2% Ru/CeO 2 catalyst exhibited good conversion of 95% and selectivity greater than 99% toward cyclohexylamine. The volcano curve describing the activity and Ru state was found. Owning to the "acidic site isolation" by surrounding alkaline sites, condensation between the neighboring amine molecules could be effectively suppressed. The catalyst also showed good stability and applicability for other aromatic amines and heteroarenes containing different functional groups.

研究领域: 催化化学 · 材料科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF POWER SOURCES · 2020 · IF 8.247

Ultrathin veil-like SnO2 supported Co3O4 nanoparticles for direct borohydride fuel cell anode

Jinfu Ma,Jing Li,Shaolin Yang,Hui Lu,Limeng Liu,Ruipeng Wang

In direct borohydride fuel cell (DBFC), there is a contradiction between catalytic activity and specific discharge capacity (SDC) owing to the dual catalytic effects of most anode catalysts on both borohydride oxidation reaction (BOR) and borohydride hydrolysis reaction (BHR). To overcome this problem, a facile method to fabricate an ultrathin tin dioxide (SnO 2 ) supported cobalt oxide (Co 3 O 4 ) composite material (u-SnO 2 /Co 3 O 4 ) as DBFC anode catalyst was developed. Both catalytic ability for BOR and specific discharge capacity of the DBFC using the u-SnO 2 /Co 3 O 4 (DBFC-u-SnO 2 /Co 3 O 4 ) with 5–10 nm thick two-dimensional (2D) SnO 2 were improved. The maximum power density (52.5 mW cm −2 ) and SDC (1380 mAh g −1 ) of DBFC-u-SnO 2 /Co 3 O 4 were respectively increased by 105% and 1740% in comparison with those of DBFC with Co 3 O 4 as anode catalyst (DBFC-Co 3 O 4 ). The u-SnO 2 /Co 3 O 4 has higher specific surface area, electron donation ability, and the rate of desorption of intermediate product (such as BH 3 OH − , H ads ) which may account for the excellent catalytic performance of u-SnO 2 /Co 3 O 4 for BOR.

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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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Improved reversible dehydrogenation properties of Mg(BH4)2 catalyzed by dual-cation transition metal fluorides K2TiF6 and K2NbF7

Jiaguang Zheng,Xuancheng Wang,Xuezhang Xiao,Hao Cheng,Liuting Zhang,Lixin Chen

Two dual-cation transition metal fluorides K 2 TiF 6 and K 2 NbF 7 are introduced into Mg(BH 4 ) 2 by ball-milling to catalyze the dehydrogenation of Mg(BH 4 ) 2 . According to the DSC and TPD results, the onset dehydrogenation temperature of Mg(BH 4 ) 2 doped with K 2 TiF 6 and K 2 NbF 7 are remarkably reduced to 105.4 and 118.0 °C, respectively. Meanwhile, both the K 2 TiF 6 and K 2 NbF 7 catalyzed systems can release more than 6.4 wt% H 2 under 280 °C, showing an improvement in dehydrogenation kinetics. In addition, the reversible capacity of the Mg(BH 4 ) 2 –3%K 2 TiF 6 system is 2.7 wt% at 280 °C in 250 min, which is enhanced comparing to that of pristine Mg(BH 4 ) 2 . X-ray diffraction, Fourier-transformed infrared and 11 B nuclear magnetic resonance investigations reveal that the K 2 TiF 6 actually acts as a catalytic precursor to react with Mg(BH 4 ) 2 , forming active hydrides of KBH 4 and TiH 2 , which further serve as catalyzing agents to facilitate the re-generation of Mg(BH 4 ) 2 from intermediates under moderate conditions.

研究领域: 材料科学 · 化学工程
✓ 已验证 DOI 高影响因子
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Advanced Membranes · 2022 · IF 0

Condensability sieving porous coordination polymer membranes for preferential permeation of C1–C4 alkanes over H2

Xuemeng Jia,De Ao,Zibo Yang,Zhihua Qiao,Yuxiu Sun,Michael D. Guiver,Chongli Zhong

Refinery gas contains abundant H 2 and a small amount of C 1 –C 4 hydrocarbons. Here, we propose a condensability sieving strategy to realize preferential permeation of hydrocarbons over H 2 by developing halogen-induced porous coordination polymer (PCP) mixed matrix membranes (MMMs) that display condensability sieving gas transport. The 4-Cl-PCP, 5-Cl-PCP and 5-Br-PCP are synthesized by using Zr 4+ and X-isophthalic acid (where X ​= ​4-Cl or 5-Cl or 5-Br) exhibit increased gas adsorption capacity with the increase in carbon number of the feed gas, but with almost no H 2 adsorption. MMMs containing the PCPs with different charge distributions enhance condensability sieving selectivity and inhibit diffusion selectivity. The permeances of the MMMs originated from condensability sieving are consistent with the polarizability-dependent adsorption of the PCP. The selectivity of the obtained MMMs for n-C 4 H 10 /H 2 , C 3 H 8 /H 2 , C 2 H 6 /H 2 , and CH 4 /H 2 achieve ∼40, ∼15, ∼5, and ∼2, respectively, exhibiting promising applications in refinery gas purification owing to their lower energy consumption compared with H 2 -preferential permeation membranes.

研究领域: 材料科学 · 化学工程 · 膜技术 · 气体分离
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2016 ·Vol. 41 ·期 15 ·6362-6368 · IF 3.205

RhNi nanocatalyst: Spontaneous alloying and high activity for hydrogen generation from hydrous hydrazine

Di-Chang Zhong,Yue-Lei Mao,Xin Tan,Ping Zhong,Liang-Xian Liu

Chemical hydrogen storage, endowed with superiorities of safety and efficiency, has been regarded as one of the most promising approaches. The design and synthesis of metallic catalytic system is an key step for development of chemical hydrogen storate materials. In this paper, we report that RhNi nanocatalyst, formed by spontaneously alloying of well-dispersed Rh and Ni NPs , exhibits much higher performance in the catalytic dehydrogenation of hydrous hydrazine.

研究领域: 材料化学 · 催化化学 · 纳米科学 · 能源化学 · 氢能源
✓ 已验证 DOI 高影响因子
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Molecular Catalysis · 2023 · IF 4.6

Facet-dependent Pd0-O2−-Ce3+ active site for selective hydrogenation of linoleate ester to cis oleic acid ester

Minghao Zha,Hao Yan,Ruiying Li,Yinghao Sun,Ruitong Wang,Yibin Liu,Xiaobo Chen,Xin Zhou,Xiang Feng,Chaohe Yang

Reducing the formation of trans fatty acid in vegetable oil hydrogenation process is of significance to ensure food safety. Herein, Pd 0 -O 2− -Ce 3+ active site was constructed by strong electronic interactions between Pd 0 and CeO 2 -Polyhedrons to promote the formation of cis fatty acid. Results reveal that the abundant oxygen vacancies of CeO 2 (111) facets promote the adsorption and activation of hydrogen, leading to excellent catalytic activity of Pd/CeO 2 -Polyhedrons. Moreover, electronic reconstructed Pd 0 -O 2− -Ce 3+ active site limits the σ-bond rotation of half-hydrogenated intermediates through enhancing π backdonation and weakening the σ-bond, contributing to the reduction of trans products. Under mild conditions (30 °C, 0.3 MPa H 2 , and 2 h), Pd/CeO 2 -Polyhedrons catalyst shows exceptional methyl oleate selectivity of 52.6% with 93.8% conversion for sunflower oil hydrogenation. The catalyst has been further extended to the selective hydrogenation to several other vegetable oils such as sunflower oil, peanut oil, soybean oil, among others, under mild conditions.

研究领域: 催化化学 · 食品安全 · 材料科学
✓ 已验证 DOI 高影响因子
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2018 · IF 11.698

In-situ synthesis of Ni2P co-catalyst decorated Zn0.5Cd0.5S nanorods for high-quantum-yield photocatalytic hydrogen production under visible light irradiation

Dongsheng Dai,Lu Wang,Nan Xiao,Songsong Li,Hao Xu,Shuang Liu,Boran Xu,Da Lv,Yangqing Gao,Weiyu Song,Lei Ge,Jian Liu

Efficient noble-metal-free semiconductor composite photocatalysts are highly desirable for visible light driven water splitting. In this study, Ni 2 P was successfully decorated on Zn 0.5 Cd 0.5 S as a highly efficient co-catalyst via a hydrothermal method . The chemical as well as photophysical properties of the as-obtained Ni 2 P/Zn 0.5 Cd 0.5 S samples were characterized by X-ray diffractometry (XRD), Transmission electron microscope (TEM), UV–vis diffusion reflectance spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), photoluminescence (PL) and time-resolved fluorescence. The Ni 2 P/ Zn 0.5 Cd 0.5 S composite sample with 4% molar content of Ni 2 P showed the highest photocatalytic H 2 evolution activity with a corresponding H 2 evolution rate of 1173 μmol h −1 , which was about 13 times higher than that of pure Zn 0.5 Cd 0.5 S sample under visible light irradiation. The photocatalytic activity of the Ni 2 P/Zn 0.5 Cd 0.5 S composite sample was stable even after 4 cycling photocatalytic experiments. A possible mechanism on the photocatalytic enhancement of the Ni 2 P/Zn 0.5 Cd 0.5 S composite sample was systematically investigated, which can provide a novel concept for the synthesis of other desirable semiconductor materials with high photocatalytic performance.

研究领域: 材料科学 · 光催化 · 能源化学 · 半导体催化 · 清洁能源
✓ 已验证 DOI 高影响因子
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

A novel hydrogen accelerated oxygen reduction Fenton reaction system: Effectively promoted the cycle of Fe(II)/Fe(III) and self-generation of H2O2

Yijun Chen,Meina Cheng,Yundong Wang,Long Jin,Juanhong Li,Hailiang Yang,Sanjian Ma,Guoliang Dai,Zixia Lin,Xin Liu

Both the iron sludge and usage of H 2 O 2 restrict the promotion of the Fenton reaction. Herein, we proposed a hydrogen-accelerated oxygen reduction Fenton reaction system named MHORF-UiO-66(Zr) to try to solve the two problems under normal temperature and pressure. The active hydrogen, which is derived from H 2 catalyzed by the composite of Pd/UiO-66(Zr), could accelerate the reduction of Fe(III) and promote the electron transfer of two-electron oxygen reduction reaction to realize the self-generation of H 2 O 2 . And 45.9 mM of H 2 O 2 could be detected. As expected, 91 % of trimethoprim (TMP) could be degraded within 30 min in this system in the condition of 25 μM Fe(II), H 2 30 mL·min −1 , and Pd/UiO-66(Zr) 2g·L −1 , which was 2.94 times that of the control Fenton system. Based on these results, the feasibility of fundamentally achieving zero emission of iron sludge was successfully verified. It was confirmed that both the hydroxyl radical and singlet oxygen played the dominant roles during the reaction process through the analysis of electron spin resonance spectroscopy. After six reaction cycles, the removal efficiency of TMP could be maintained at least 94 %. It found that both the properties and morphology of this composite could remain based on the systematic characterization.

研究领域: 环境科学 · 化学工程 · 催化材料
✓ 已验证 DOI 高影响因子
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FUEL · 2023 · IF 7.4

MoS2 catalysts with adjustable size and layer structure derived from polyoxometalates-ionic liquids complexes for hydrogen production and hydrogenation

Zekun Guan,Minmin Wang,Guangxun Sun,Xin Xue,Yanfei Chen,Yu Zhang,Ting Zhao,Hongfu Shi,Chao Feng,Yuan Pan,Yunqi Liu

In the period of energy conversion, the effective utilization of fossil fuels and the development of new energy sources are becoming extremely imperative. MoS 2 have excellent catalytic activity for fuel hydrogenation and hydrogen production. However, the synthesis of highly dispersed MoS 2 that can expose more active sites has been challenging. Herein, (DODA) 6 Mo 7 O 24 with organic–inorganic core–shell structure was prepared by POMs-ILs (polyoxometalates-ionic liquids) self-assembly. MoS 2 with adjustable size and layer structure derived from (DODA) 6 Mo 7 O 24 by controllable confined-sulfidation effect for hydrogenation and hydrogen evolution reaction (HER). Among them, MoS 2 (T 280 S 1:4 t 30 ) has the lowest overpotential, and only 200 mV is needed to reach the current density of 10 mA·cm −2 . At the same time, it has the optimal hydrogenation performance with the highest selectivity for octahydroanthracene and perhydroanthracene, along with a hydrogenation percentage of 48.04 % in the process of anthracene hydrogenation. Density functional theory demonstrated that the monolayer MoS 2 was more favorable for water molecule dissociation and hydrogen molecule activation, which proves that the MoS 2 has excellent catalytic activity for HER and hydrogenation simultaneously. This work is instructive for the synthesis of MoS 2 and its application in HER and hydrogenation.

研究领域: 能源材料化学 · 催化化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2022 · IF 6.76

Construction of polysulfone anion exchange hybrid membranes by incorporating carbon quantum dots and facilitated transport mechanisms

Yuan Jin,Xiu Zhang,Tianci Feng,Meisheng Li,Huifang Xiao,Shouyong Zhou,Yijiang Zhao,Jing Zhong,Dawei Yang

Low ion conductivity and poor alkali resistance are still the two major obstacles for the applications of anion exchange membranes (AEMs). In this work, the combined strategies of Carbon quantum dots (CQDs) hybrid and cross-linking modification via side-chains designing were employed to prepare organic–inorganic hybrid AEMs. Then, the cross-linked quaternized polysulfone (CQPSf-CQDs) hybrid AEMs by incorporating carbon quantum dots were successfully fabricated. After hybrid and cross-linking, the mechanical properties of CQPSf-CQDs hybrid AEMs were higher than that of the pristine one, reaching 49.4 MPa for the best one. Meanwhile, the existence of CQDs can expand the hydrophilic area in the membrane, which is beneficial to the transport of O H - . The incorporated CQDs interact weakly with cationic groups in the side chains through hydrogen bonds. The simulation results further demonstrated that the introduction of CQDs was beneficial to the construction of hydrophilic and hydrophobic domains, thereby increasing O H - conductivity. In addition, the prepared hybrid membranes own excellent dimensional stabilities and ion transport performances. These preliminary results give us a lot of hopes for further experiments and optimizations for the hybrid AEMs.

研究领域: 材料科学 · 高分子化学 · 膜科学与技术 · 电化学 · 能源材料
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