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Frontiers in Energy · 2024 ·Vol. 18 ·期 3 ·378-389 · IF 3.1

Two-dimensional bimetallic selenium-containing metal-organic frameworks and their calcinated derivatives as electrocatalysts for overall water splitting

Shang Zhao-ting,Li Tang-ming,Hu Bing-qian,Liu Min,Lu Wang-ting,Yu Fan,Zheng Yun

The use of two-dimensional (2D) layered metal-organic frameworks (MOFs) as self-sacrificial templates has been proven to be a successful method to create high-efficiency Selenium (Se)-containing electrocatalysts for overall water splitting. Herein, two strategies are then utilized to introduce Se element into the Co–Fe MOF, one being the etching of as-prepared MOF by SeO 2 solution, and the other, the replacing of SCN − with SeCN − as the construction unit. The electrochemical activity of the pristine 2D MOF and their calcinated derivatives for catalyzing the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is evaluated and further discussed. It is found that the effect of introducing Se on improving electrochemical catalytic activity is significant for the HER process. Specifically, the calcinated derivative in the replacing method exhibits an overpotential of 235 mV for HER and 270 mV for OER at a current density of 10 mA/cm 2 . For comparing the two methods of introducing Se element into MOF, similar electrocatalytic activity can be achieved on the their calcinated derivatives. The high electrochemical performance of 2D CoFe-MOF derivatives may be resulted from the unique 2D hierarchical porous structure and strong synergistic effect between different components in the material.

研究领域: 材料科学 · 电化学 · 纳米技术 · 催化 · 能量转换
✓ 已验证 DOI 高影响因子
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RARE METALS · 2023 ·Vol. 42 ·期 12 ·3993-4004 · IF 8.8

2D-MOF/2D-MOF heterojunctions with strong hetero-interface interaction for enhanced photocatalytic hydrogen evolution

Ma Yan,Fang Hui-Xue,Chen Rong,Chen Qian,Liu Sheng-Jun,Zhang Kui,Li Hai-Jin

Metal organic framework (MOF) shows great potential in the research field of photocatalysis, and it is a big challenge to achieve efficient photocatalytic activity. In this work, we have successfully grown two-dimensional MOF (2D-MOF) nanosheets on 2D-MOF nanosheets for the first time using a homometallic nodal strategy, and successfully prepared ultrathin nanosheets with tightly bound 2D/2D heterojunctions. 2D Ni-BDC nanosheets were used as carriers to grow 2D Ni-TCPP nanosheets on top of them. Ni-TCPP has a high light absorption capacity, thus extending the light absorption range of 2D/2D heterojunctions. The tight coupling of the heterojunction effectively shortens the electron transfer distance, promotes the separation of interfacial charges, and improves the photocatalytic activity. Particularly, Ni-BDC/Ni-TCPP-3 can achieve to a hydrogen production rate of 428.0 μmol·g −1 , approximately 5.75 times higher than Ni-BDC and 5.24 times higher than Ni-TCPP, respectively. Thus, 2D-MOF/2D-MOF heterojunctions provide a promising strategy for enhancing photocatalytic performance through rational heterostructure design with homometallic node strategy. Graphical abstract

研究领域: 材料科学 · 纳米技术 · 催化 · 能量转换
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Small · 2022 ·Vol. 18 ·期 45 ·2204255 · IF 15.153

Convex Cube-Shaped Pt34Fe5Ni20Cu31Mo9Ru High Entropy Alloy Catalysts toward High-Performance Multifunctional Electrocatalysis

Zhaoqian Chen,Jingbo Wen,Chaohui Wang,Xiongwu Kang

High entropy alloy (HEA) catalysts exhibit excellent multifunctional catalytic performance due to the synergistic effect of multi-metal components. However, shape-controlled synthesis of such kinds of HEA catalysts, especially those with high index facets, still faces great challenges, limiting further enhancement of their catalytic performance. Herein, one-pot synthesis of convex cube-shaped Pt 34 Fe 5 Ni 20 Cu 31 Mo 9 Ru HEA catalysts which possess rich (310) facets and a diagonal crystalline size of 38.5 nm is reported. Transmission electron microscopy measurements indicate cube-shaped nanocrystals are obtained first and further selective growth of pyramid on each facet of the cube-shaped nanocrystal results in a convex cube shape. Pt 34 Fe 5 Ni 20 Cu 31 Mo 9 Ru HEA catalysts show excellent electrocatalytic performance toward the oxygen reduction reaction (ORR), hydrogen evolution reaction (HER), and oxygen evolution reaction (OER), which exhibit a half-wave potential of 0.87 V for ORR in 0.1 m HClO 4 , and overpotential of 20 and 259 mV for HER and OER at a current density of 10 mA cm −2 in an alkaline medium. A control experiment and density functional theory calculation indicate that the Ru element plays a decisive role in both the formation of the convex cube shape and also the high catalytic performance.

研究领域: 材料科学 · 电催化 · 理论计算
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Both MOFs-derived Fe-Co-Ni ternary hydroxide positive and Fe2O3/reduced graphene oxide negative electrode for asymmetric supercapacitors

Mohan Huang,Kun Zhao,Zhiying Bai,Dawei He,Jiaqi He,Yongsheng Wang

To design and construct high-performance asymmetric supercapacitors (ASC), we use the same Fe-based metal-organic framework (MIL-88A) as the precursor for the first time to prepare iron-cobalt-nickel ternary metal hydroxides (Fe-Co-Ni-OH) and Fe 2 O 3 compounded with reduced graphene oxide (Fe 2 O 3 /RGO-1). As a positive electrode, Fe-Co-Ni-OH has a specific capacitance of 1065 F g −1 at 1 A g −1 and exhibits excellent rate performance and cycle stability due to its unique spindle-like structure of the surface growth nanosheets and the synergistic effect between the three metals. The introduction of RGO effectively connects the independent spindle-like Fe 2 O 3 and enhances the conductivity and structural stability of the material. So that the Fe 2 O 3 /RGO-1 negative electrode has a specific capacitance of 734 F g −1 at 1 A g −1 , and its cycle stability is significantly improved compared with the single Fe 2 O 3 (increasing from 64 % to 85 %). The constructed Fe-Co-Ni-OH//Fe 2 O 3 /RGO-1 ASC possesses a satisfactory energy density of 43.11 Wh kg −1 at a power density of 800 W kg −1 , which is superior to parts constructed with similar material compositions in the same period. This research provides a new perspective for developing high-performance, low-cost, and environmentally friendly green energy storage devices.

研究领域: 材料科学 · 能源存储技术
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MICROCHEMICAL JOURNAL · 2022 · IF 5.304

Quantitative evaluation of human carboxylesterase 1 by SERS-ELISA using a synergistic enhancement strategy based on gold nanoparticles and metal–organic framework

Hao Lu,Yu Yang,Ruijue Chen,Wenyi Huang,Hao Cheng,Xueping Liu,Hongxing Kong,Lijun Li,Jun Feng

In this study, we synthesized gold nanoparticles (AuNPs) in situ on the surface of two-dimensional Cu-TCPP (meso-tetra(4-carboxyphenyl)porphine) metal– organic framework (MOF) nanosheets to produce AuNP@Cu-TCPP nanocomposites as surface-enhanced Raman scattering (SERS) substrates. The SERS signal was enhanced in two ways: aggregation of the AuNPs@Cu-TCPP near the SERS hotspot through the strong adsorption capacity of the MOF, and the synergistic effect between the charge-transfer enhancement of the Cu-TCPP MOF and the electromagnetic enhancement of plasmonic metal AuNPs. The SERS activity of AuNPs@Cu-TCPP was evaluated by the analysis of multiple model analytes; Rhodamine 6G (R6G) and benzidine were detected with detection limits below 10 –13 and 10 –12 mol·L –1 , respectively. We used AuNP@Cu-TCPP as a SERS substrate combined with an enzyme-linked immuno- sorbent assay (ELISA) to detect the tumor marker carboxylesterase 1 (hCE1) in human serum. The SERS signal of benzidine at 1609 cm −1 is linearly correlated with hCE1 in the concentration range of 0.1–120 ng·mL −1 . Owing to their high sensitivity and excellent SERS sensing capability, AuNPs@Cu-TCPP nanocomposites have potential applicability in the analysis of clinical samples.

研究领域: 生物医学工程 · 分析化学 · 肿瘤标志物检测
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ACS Catalysis · 2016 · IF 9.307

Synergistic Effects of Au and FeOx Nanocomposites in Catalytic NO Reduction with CO

Xianwei Wang,Nobutaka Maeda,Alfons Baiker

Promotion of Au/TiO2 by FeOx addition is shown to result in a very strong enhancement of activity and selectivity in the NO reduction with CO. The nanocomposite Au-FeOx/TiO2 catalysts were prepared by deposition–precipitation (Au/TiO2) and subsequent impregnation (FeOx). Structural characterization of the nanocomposite catalysts using XRD, TEM, TPR, XPS, and DRIFTS revealed that they consist of titania-supported Au particles of about 4.4–4.8 nm size, which were partially covered with a thin layer of FeOx,, mainly made up of Fe2+ (FeO), in addition to a small fraction of Fe3+ (Fe2O3). In situ DRIFTS studies showed that, in comparison to Au/TiO2, on the Au-FeOx/TiO2 nanocomposites new adsorption sites were created, which led to enrichment of CO and NO molecules on the Au surface and at its interfaces with FeOx and TiO2. At the reaction temperature (250 °C), a new surface NO–CO complex, where both Fe and Au are proposed to be involved in the adsorptive interaction, was discovered. The titania-supported Au-FeOx nanocomposites considerably facilitated the formation of this complex and contributed to the striking enhancement of the catalytic performance (activity and selectivity) of the Au-based catalyst.

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 MATERIALS ENGINEERING AND PERFORMANCE · 2020 ·Vol. 29 ·期 11 ·7239-7249 · IF 1.652

Dissimilar Metal Joining of Ti and Ni Using Ti-Al Powder Interlayer Via Rapid Thermal Explosion Method

Sang Changcheng,Cai Xiaoping,Zhu Lu,Ren Xuanru,Niu Gao,Wang Xiaohong,Feng Peizhong

To achieve the low energy consumption and high strength joining between Ti and Ni, a novel joining method (rapid thermal explosion, TE) was developed for joining dissimilar metals using Ti-Al mixture powders as flux. The TE reaction temperature of Ti-Al flux was measured, and the microstructure and mechanical properties of Ti/Ni joint were investigated. The results reveal that the combustion temperature of the Ti-Al powder interlayer is 1103 °C, which is higher than the joining temperature, and an obvious self-exothermic phenomenon lasts 20 s. The intermetallic compound diffusion layers formed at both interfaces mainly owing to the diffusion of Al and the growth activation energy of diffusion layers near both interfaces are 79.68 kJ/mol and 38.26 kJ/mol, respectively. Based on the sheer strength and diffusion layer, the formation mechanism of Ti/Ni joints is metallurgical bonding through atomic diffusion and formation of the diffusion layer.

研究领域: 材料科学 · 焊接工程 · 金属间化合物 · 界面化学 · 固态连接
✓ 已验证 DOI 高影响因子
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DALTON TRANSACTIONS · 2023 ·Vol. 52 ·期 11 ·3351-3357 · IF 4

In situ artificial solid electrolyte interface engineering on an anode for prolonging the cycle life of lithium-metal batteries

Keke Shen,Di Wang,Xinzhi Ma,Kaixin Zhao,Qi Jin,Junpeng Xiao,Yong Cai,Yufei Zhang,Lili Wu,Xitian Zhang

Lithium, with its high theoretical capacity and low potential, has been widely investigated as the anode in energy storage/conversion devices. However, their commercial applications always suffer from undesired dendrite growth, which forms in the charging process and may puncture the separator, leading to short cycle lives and even security problems. Herein, by an in situ displacement reaction using SnF2 at room temperature, we constructed an artificial solid electrolyte interface (ASEI) of LiF/Li–Sn outside the Li anode. This hybrid strategy can induce a synergy between the high Li+ conductivity of the Li–Sn alloy and good electrical insulation of LiF. Moreover, extreme synergy can be achieved by moderating the thickness of the LiF/Li–Sn ASEI, guiding dendrite-free lithium plating and stripping. As a result, a Li//LiFePO4 battery that is assembled from the LiF/Li–Sn ASEI-engineered Li anode can obtain 1000 cycled lives with 86.3% capacity retention under a charge/discharge rate of 5 C. This work provides an alternative way to construct dendrite-free lithium metal anodes, which significantly benefit the cycle lives of LMBs.

研究领域: 电化学 · 材料科学 · 能源存储 · 纳米材料 · 界面化学 · 电池技术
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE · 2024 ·Vol. 59 ·期 6 ·2302-2314 · IF 3.5

Deposition of Pd–Pt alloy zigzag shell over Au nanorods for boosted catalysis and thermo-photo catalysis

Dou Yun-Qi,Zhang Qi,Deng Tian-Song,Cheng Zhiqun,Zhao Xiaoyu

Multimetallic plasmonic nanostructures, with appropriate morphology, elemental proportions and sizes, can be used to accelerate photocatalytic reactions. Here, we designed zigzag trimetallic nanostructures with the Au core and Pd–Pt alloy shell, whose catalytic ability was boosted by the synergistic effect of the plasmonic metal and catalytic metal. The catalytic rate of Au@PdPt nanoparticle (NP) with no light have a significant improvement, attributed to the larger contact area provided by the zigzag alloy shell. Furthermore, the enhanced catalytic activity in the presence of light is primarily due to the thermo-photo catalytic effect of plasmonic Au. The adding ratios of Pd:Pt were adjusted from 1:4 to 4:1, and we found that, when adding the Pd:Pt of 1:1, the zigzag Au@PdPt nanoparticle (NP) exhibited a superior reaction rate in the reduction methylene blue (MB) under light illumination. The rate is 8 times higher than that of Au@Pt, and the reduction conversion reached 100%. And it has a favorable plasmon enhancement factor with an appropriate shell thickness and get the balance between the catalytic performance and economic effects. This structure driven by capability-oriented design principles and holds the potential for applications in the field of catalysis. Graphical abstract

研究领域: 纳米技术 · 催化 · 材料科学 · 等离激元学 · 化学工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2017 · IF 3.133

Improved electrochemical performance of Ti1.4V0.6Ni hydrogen storage alloy in its composite with LiAlH4

Jing Lin,Zhanyi Cao,Lianshan Sun,Fei Liang,Limin Wang

Ti 1.4 V 0.6 Ni +  x LiAlH 4 ( x  = 0.5, 1, 1.5, 2, 2.5, wt.%) composites were prepared by ball-milling, and the effects of LiAlH 4 content on structure and electrochemical properties of the composites were investigated systematically. The addition of LiAlH 4 to the Ti 1.4 V 0.6 Ni alloy significantly affected the morphology and size of the composite particles . The electrochemical cycling stability and rate dischargeability of the composite electrodes benefitted from adding some LiAlH 4 ( x  = 1), which however deteriorated when the LiAlH 4 content increased further. The positive effect of LiAlH 4 on the electrochemical performance of the studied alloy was caused by suppression of the dissolution of active components of the Ti 1.4 V 0.6 Ni hydrogen storage alloy.

研究领域: 材料科学 · 金属功能材料 · 能源存储 · 电化学 · 氢能技术
✓ 已验证 DOI 高影响因子
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RSC Advances · 2017 ·Vol. 7 ·期 72 ·45420-45431 · IF 3.108

High efficiency and stability of Au–Cu/hydroxyapatite catalyst for the oxidation of carbon monoxide

Jiuli Guo,Huanhuan Yu,Feng Dong,Baolin Zhu,Weiping Huang,Shoumin Zhang

A highly efficient and stable Au–Cu/hydroxyapatite (HAP, Ca10(PO4)6(OH)2) catalyst was reported. HAP was prepared through a deposition–precipitation method. Au–Cu/HAP catalysts were obtained by a two-step impregnation approach. The samples were characterized by XRD, TEM, SEM, UV-Vis, ICP, XPS, H2-TPR, and O2-TPD. CO oxidation reaction was carried out to evaluate the catalytic performance of samples. TEM and UV-Vis results showed that the metallic particles supported on Au–Cu/HAP were smaller than those on Au/HAP, and they were highly dispersed on the HAP support. Patterns of XPS revealed that CuO nanoparticles were formed in the Cu/HAP catalyst, while CuO and Cu2O species coexisted in Au–Cu/HAP catalyst. Based on the O2-TPD data, the addition of copper to Au/HAP gave rise to more new O2 adsorption sites and bigger O2 adsorption capacity. The catalysis results indicated that the Au–Cu/HAP was capable of obtaining higher efficiency and stability compared with Au/HAP and Cu/HAP for CO oxidation. It was likely that the synergistic interaction between gold and CuOx phase created the most active sites on Au–Cu/HAP and was responsible for the enhanced activity and stability in comparison with Au/HAP and Cu/HAP.

研究领域: 催化化学 · 材料科学 · 环境化学 · 纳米催化 · 表面科学
✓ 已验证 DOI 高影响因子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Development of a magnetic calcium-alginate hydrogel-sphere encapsulated with Fe–Mn–Zr ternary metal composite for heavy metal adsorption

Baicheng Yuan,Xinyi Huang,Shaojinlin Yang,Yi Yang,Zhihong Lin,Raphael Semiat,J. Paul Chen

Heavy metal contamination has become one of the greatest global environmental problems. In this study, a magnetic calcium-alginate hydrogel-sphere encapsulated with Fe–Mn–Zr ternary-metal composite (MCHETC) was prepared through a combined co-precipitation and extrusion approach and used for the adsorption of heavy metals in aqueous solutions. The active sites were dispersed in the MCHETC, which can be separated by the magnetic force for the ease in operation. Above 80% of ultimate adsorption was completed at a contact time of 5 h. The copper uptake history was well described by the intraparticle surface diffusion model, suggesting a multi-step process for the adsorption. The optimum pH for adsorption was 4; the maximum adsorption capacity was 103.1 mg-Cu/g. The adsorption capability well remained after the 5 adsorption–desorption cycles and the copper could be recovered. Furthermore, the adsorbent performed well in the nature water spiked with copper ions. The mechanism studies illustrated that the adsorption was mainly controlled by the ion-exchange reaction. This study demonstrated that the MCHETC adsorption technology may be used for heavy metal removal and recovery with higher efficacy.

研究领域: 环境科学 · 材料科学
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