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CommunicationAnion-templated Self-assembly for the Preparation of Silver-t-butylthiolate ClustersJIN Jun-Ling, SHEN Yang-Lin, MI Li-Wei*, XIE Yun-Peng* and LU Xing*
Chin. J. Struct. Chem. 2022, 41, 2203100-2203107 DOI: 10.14102/j.cnki.0254-5861.2011-3357
March 15, 2022
silver cluster, X-ray crystal structure, silver thiolate polymer, self-assembly
ABSTRACT
Silver thiolate polymers are intercepted to form different structural fragments when reacting with variant solubilizing reagents, which usually serve as the starting point for the preparation of clusters. However, such a process is still far from clear. Herein, we report the controlled synthesis of silver-t-butylthiolate clusters from reactions of polymeric [AgtBuS]n and suitable templates in the presence of solubilizing reagents to offer a detailed look at the mechanism of cluster’s formation. As the provided solubilizing reagents have weak coordination ability, such as O- or N-donating ligands, the obtained polymeric compound retains the linear structure pattern that S and Ag atoms are arranged alternately. When extra templates NO3− and CO32− are applied, the disk-like clusters Ag19 and Ag20 are constructed with the same [AgtBuS]5 circles that may directly cyclize from the linear [AgtBuS]n fragments. In contrast, (EtO)2PS2− and (iPrO)2PS2− anions have large size and strong coordination ability rendering the structure of the polymer completely fragmented. Thus extremely short [AgtBuS]n pieces with silver ions and solubilizing ligands assemble around the templates V2O74− and W2O94−, leading to the formation of clusters Ag22 and Ag24. -
ArticleMOF-Conductive Polymer Composite Film as Electrocatalyst for Oxygen Reduction in Acidic MediaZHUGE Rui-Xue, SHI Peng-Chao and ZHANG Teng*
Chin. J. Struct. Chem. 2022, 41, 2203062-2203069 DOI: 10.14102/j.cnki.0254-5861.2011-3350
March 15, 2022
metal-organic frameworks (MOFs), conductive polymer, porphyrin, oxygen reduction reaction (ORR), electrocatalysis
ABSTRACT
A metal-organic framework (MOF)-conductive polymer composite film was constructed from PCN-222(Fe) nanoparticles and PEDOT:PSS solution by simple drop-casting approach. The composite film was tested as an electrocatalytic device for oxygen reduction reaction (ORR). The combination of PCN-222(Fe) MOF particles and conductive PEDOT matrix facilitates electron transfer in the composite material and improves the ORR performance of PCN-222(Fe). Levich plot and H2O2quantification experiment show that PCN-222(Fe)/PEDOT:PSS film mainly catalyzes two-electron oxygen reduction and produces H2O2.
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ArticleNi(OH)2 Derived from NiS2 Induced by Reflux Playing Three Roles for Hydrogen/oxygen Evolution Reaction
Sheng-Jun Xu*, Ya-Nan Zhou, Guo-Ping Shen and Bin Dong*
Chin. J. Struct. Chem. 2022, 41, 2208052-2208057 DOI: 10.14102/j.cnki.0254-5861.2022-0143
July 25, 2022
Ni(OH)2, NiS2, heterostructures, oxygen evolution reaction, hydrogen evolution reaction
ABSTRACT
Developing efficient and promising non-noble catalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is vital but still a huge challenge for the clean energy system. Herein, we have integrated the active components for OER (Ni(OH)2) and HER (NiS2 and Ni(OH)2) into Ni(OH)2@NiS2 heterostructures by a facile reflux method. The in-situ formed Ni(OH)2 thin layer is coated on the surface of hollow NiS2 nanosphere. The uniform Ni(OH)2@NiS2 hollow sphere processes enlarge the electrochemically active specific surface area and enhance the intrinsic activity compared to NiS2 precursor, which affords a current density of 10 mA cm-2 at the overpotential of 309 mV and 100 mA cm-2 at 359 mV for OER. Meanwhile, Ni(OH)2@NiS2 can reach 10 mA cm-2 at 233 mV for HER, superior to pure NiS2. The enhanced performance can be attributed to the synergy between Ni(OH)2 and NiS2. Specifically, Ni(OH)2 has three functions for water splitting: providing active sites for hydrogen adsorption and hydroxyl group desorption and working as real OER active sites. Moreover, Ni(OH)2@NiS2 displays great stability for OER (50 h) and HER (30 h).
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ArticleCo-Construction of Sulfur Vacancies and Heterogeneous Interface into Ni3S2/MoS2 Catalysts to Achieve Highly Efficient Overall Water SplittingZhaoyang An, Hui Xue*, Jing Sun, Niankun Guo, Tianshan Song, Jiawen Sun, Yi-Ru Hao and Qin Wang*
Chin. J. Struct. Chem. 2022, 41, 2208037-2208043 DOI: 10.14102/j.cnki.0254-5861.2022-0130
July 25, 2022
sulfur vacancies, heterostructures, transition metal chalcogenides, overall water splitting
ABSTRACT
Integrating the advantages of anion vacancies and heterostructures into the catalytic materials may increase the binding affinities to intermediates, provide more active sites, and significantly promote the activity of overall water splitting. However, the successful assembly of anion vacancies and heterostructures for high-efficiency water splitting performance is still challenging. In this work, we ingeniously present the co-construction of sulfur vacancies and heterogeneous interface into Ni3S2/MoS2 catalysts on nickel foam (NF). The introduction of sulfur vacancies and Ni3S2/MoS2 heterostructures can significantly improve electron and ion transport, effectively improve structural stability, and enhance overall water splitting activity. The obtained VS-Ni3S2/MoS2 catalysts (VS stands for sulfur vacancies) exhibit superior OER and HER activities, and the overpotentials for OER and HER are 180 and 71 mV at 10 mA·cm-2, respectively. Furthermore, a low water splitting voltage of 1.46 V is required at 10 mA·cm-2 for the VS-Ni3S2/MoS2 catalysts, which is considerably lower than most of the water splitting electrocatalysts currently reported. This work offers an effective mean for the preparation of catalysts with both anion vacancies and heterostructures for achieving high-performance alkaline overall water splitting. -
ArticleEnhanced Photocatalytic H2-production Activity of CdS Nanoflower using Single Atom Pt and Graphene Quantum Dot as Dual Cocatalysts
Yi Yang, Jinsong Wu, Bei Cheng*, Liuyang Zhang*, Ahmed Abdullah Al-Ghamdi, Swelm Wageh and Youji Li
Chin. J. Struct. Chem. 2022, 41, 2206006-2206014 DOI: 10.14102/j.cnki.0254-5861.2022-0124
June 20, 2022
hierarchical nanostructure, single-atom catalysts, graphene quantum dots, CdS nanosheets, hydrogen production
ABSTRACT
Single-atom catalysts have high catalytic activity due to their unique quantum size effects and optimal atom utilization. Herein, visible-light-responsive photocatalysts were designed by coupling CdS with graphene quantum dots (GQDs) and platinum single atoms (PtSAs). GQDs and PtSAs were successively loaded on ultrathin CdS nanosheets through freeze-drying and in-situ photocatalytic reduction. The synergistic effect between PtSAs and GQDs results in superior photocatalytic activity with a hydrogen production rate of 13488 μmol h-1 g-1 as well as the maximum apparent quantum efficiency (AQE) of 35.5% in lactic acid aqueous solution, which is 62 times higher than that of pristine CdS (213 μmol g-1 h-1). The energy conversion efficiency is ca. 13.05%. As a photosensitizer and an electron reservoir, GQDs can not only extend the light response of CdS to the visible-light region (400-800 nm), but also promotes the separation of photoinduced electron-hole pairs. Meanwhile, PtSAs, with unique electronic and geometric features, can provide more efficient proton reduction sites. This finding provides an effective strategy to remarkably improve photocatalytic H2 production performance. -
Short CommunicationFlexible Organic Single Crystal with Elastic Bending and Plastic Twisting Capabilities
Jiang Peng†*, Wanjun Zhao†, Jing Zhang, Chuchu Han, Junhui Jia, Tingting Feng and Jiawen Sun
Chin. J. Struct. Chem. 2022, 41, 2212004-2212006 DOI: 10.14102/j.cnki.0254-5861.2022-0217
December 2, 2022
flexible crystal, elastic bending, plastic twisting, elastoplastic deformation, waveguide
ABSTRACT
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ArticleExplicating the Role of Metal Centers in Porphyrin-Based MOFs of PCN-222(M) for Electrochemical Reduction of CO2
Mengjie Liu, Mengting Peng, Baoxia Dong*, Yunlei Teng, Ligang Feng and Qiang Xu*
Chin. J. Struct. Chem. 2022, 41, 2207046-2207052 DOI: 10.14102/j.cnki.0254-5861.2022-0057
July 18, 2022
PCN-222, electrochemical reduction of CO2, DFT calculation, MOFs
ABSTRACT
The porphyrin-based MOFs formed by combining Zr6 clusters and porphyrin carboxylic acids with clear M-N4 active centers show unique advantages in electrocatalytic reduction of CO2 (CO2RR). However, its conductivity is still the bottleneck that limits its catalytic activity due to the electrical insulation of the Zr cluster. Therefore, the porphyrin-based MOFs of PCN-222(M) (M = Mn, Co, Ni, Zn) with explicit M-N4 coordination were combined with the highly conductive material carbon nanotube (CNT) for discussing the influence of metal centers on the CO2RR performance based on theoretical calculations and experimental observations. The results show that the PCN-222(Mn)/CNT, PCN-222(Co)/CNT, and PCN-222(Zn)/CNT all exhibit high selectivity to CO (FECO > 80%) in the range of -0.60 to -0.70 V vs. RHE. The FECOmax of PCN-222(Mn)/CNT (-0.60 V vs. RHE), PCN-222(Co)/CNT (-0.65 V vs. RHE), and PCN-222(Zn)/CNT (-0.70 V vs. RHE) are 88.5%, 89.3% and 92.5%, respectively. The high catalytic activity of PCN-222(Mn)/CNT and PCN-222(Co)/CNT comes from the excellent electron mobility of their porphyrin rings and their low ΔG*COOH (0.87 and 0.58 eV). It reveals that the strength of backbonding π of the transition metal and its influence on the electron mobility in the porphyrin ring can affect its CO2RR activity. -
ArticleTemperature-controlled Structural Diversity of Two Cd(II) Coordination Polymers Based on the Dicarboxylate LigandCHEN Fang-Min, ZHOU Chi-Chi, HE Xiong, LI Yan* and ZHANG Xiu-Qing*
Chin. J. Struct. Chem. 2022, 41, 2202014-2202022 DOI: 10.14102/j.cnki.0254-5861.2011-3234
February 15, 2022
Cd(II) coordination polymers, p-phthalic acid, Hirshfeld surface, Luminescent properties
ABSTRACT
Two new 3-D Cd(II) coordination polymers with p-phthalic acid (p-BDC) and 4,4΄-dipyridyl-amine (4,4΄-dpa), namely [Cd2(p-BDC)2(4,4΄-dpa)2]n 1 and {[Cd(p-BDC)(4,4΄-dpa) (H2O)]·4H2O}n 2 were successfully synthesized under hydrothermal conditions at 120 and 140 °C. They were characterized by single-crystal X-ray diffraction, IR, PXRD and TGA. It was further characterized by Hirshfeld surface (HS) analysis for complex 2. The luminescent properties of the complexes have also been investigated. -
LetterA Terbium(III)-organic Coordination Polymer: Synthesis, Characterization and Its LuminescenceMI Ying-Hao, YANG Ming-Xue, KUANG Xiao-Fei* and LU Can-Zhong*
Chin. J. Struct. Chem. 2022, 41, 2202079-2202084 DOI: 10.14102/j.cnki.0254-5861.2011-3277
February 15, 2022
coordination polymer, crystal structure, photoluminescence
ABSTRACT
A new 3D terbium(III) metal-organic network [Tb(HIMDC)(HCOO)(H2O)]n (complex 1) has been synthesized by Tb3+ ions coordinated with 4,5-imidazole dicarboxylic acid (H3IMDC) and formic acid under solvothermal conditions with the mixed solvents of N,N-dimethylformamide (DMF) and H2O. The unambiguous structural determination has been confirmed by single-crystal X-ray diffraction combined with elemental analysis, infrared (IR) spectrum, thermogravimetric analysis (TGA) and powder X-ray diffraction (PXRD). Complex 1 crystallizes in orthorhombic Fdd2 space group with a = 22.295(2), b = 24.097(3), c = 6.7256(6) Å, V = 3613.3 Å3, Z = 16, Dc = 2.765 g/cm3, F(000) = 2816, μ = 7.855 mm-1, the final R = 0.0173 (I ≥ 2σ(I)), wR = 0.0416 (all data) and GOOF = 1.068. In complex 1, the Tb3+ ions are connected by HIMDC2- anions into 2D metal-organic layers which are further extended into a three-dimensional (3D) architecture through formic acid functional motif. In addition, complex 1 shows intense and characteristic green luminescence. -
CommunicationSynthesis, Crystal Structure and Fluorescent Properties of a 1D Europium Coordination Polymer with 2,5-Furandicarboxylic AcidZHANG Han, LI Xiang, MUHAMMAD Yaseen, XIE Hui-Feng, ZANG Yi-Han, FANG Ming-Lu, LIU Shao-Jie and WANG Hao*
Chin. J. Struct. Chem. 2022, 41, 2203092-2203099 DOI: 10.14102/j.cnki.0254-5861.2011-3303
March 15, 2022
2,5-furandicarboxylic acid, solvothermal synthesis, Fe3+, fluorescence quenching
ABSTRACT
By using solvothermal method, a one-dimensional chain compound [KEu2(FDCA)3(H2O)9·0.5(FDCA)] (1) was synthesized. Single-crystal X-ray diffraction data reveal that 1 crystallizes in monoclinic system, space group P21/n with a = 12.1996(1), b = 18.6454(2), c = 17.7123(2) Å, β = 98.8460(10)°, Dc = 1.753 g/cm3, Z = 2, V = 3981.03(7) Å3, R = 0.0544 and wR = 0.1511 for 7886 observed reflections with I > 2σ(I). In 1, three FDCA2– ligands construct a “23-crown-9-like” structure as the second building units (SBUs) to further form an infinite 1D chain. Meanwhile, the fluorescent result reveals that compound 1 can selectively and sensitively sense Fe3+ by the fluorescence quenching. -
Morphology Engineering toward Highly Emissive Mn2+ Doped PEA2PbBr4 Perovskite with Their LED Application via Phosphonium PassivationYu-Feng Sang, Liang-Jin Xu* and Zhong-Ning Chen*
Chin. J. Struct. Chem. 2022, 41, 2205070-2205076 DOI: 10.14102/j.cnki.0254-5861.2022-0088
May 20, 2022
2D perovskite, Mn2+ doped, energy transfer, perovskite LED
ABSTRACT
Mn2+-doped lead halide perovskites either in 3D or 2D have been extensively explored due to their rich energy-transfer behaviors. While their application on LED is still lagging behind in comparison to non-doped 3D perovskite due to inferior film-formation and low luminescent efficiency. Here we report an in-situ-formed Mn2+ doped 2D perovskite nanocrystal (NCs) film by introducing quaternary phosphonium salt during the crystallizing process. The as-formed film shows improved luminescent efficiency with emission peaked at 600 nm and photoluminescence quantum yield (PLQY) of as high as 73.37%, which is about 1.3 times higher than that of pristine film. Further characterizations confirm the enhanced confinement effect from smaller size particle is responsible for the improved luminescent efficiency. The perovskite LEDs based on pristine and phosphonium passivated thin films were fabricated, and a great improvement in the external quantum efficiency of these LEDs (from 0.0017% to 0.12%) is observed due to the improved morphology and enhanced luminescent efficiency. -
ArticleSelective Electrocatalytic Hydrogenation of 5-Hydroxymethyl-furfural to 2,5-Dihydroxymethylfuran on Bimetallic PdCu Alloy
Xu Yue, Weixing Zhao, Shuangyin Wang and Yuqin Zou*
Chin. J. Struct. Chem. 2022, 41, 2205063-2205069 DOI: 10.14102/j.cnki.0254-5861.2022-0074
May 20, 2022
biomass, 2,5-dihydroxymethylfuran, electrocatalyst, bimetallic alloy, hydrogenation
ABSTRACT
2,5-Dihydroxymethylfuran (DHMF), obtained from 5-hydroxymethylfurfural (HMF) by electrochemical method, is a promising building block for polymers. However, one challenge of this process is to reduce initial potential and improve catalytic selectivity. In this work, the PdCu bimetallic catalyst is prepared with an onset potential of -0.05 VRHE and a selectivity of 99%. Compared with the single Cu electrocatalyst, the adsorption of HMF and proton is improved by introducing of Pd, which is demonstrated by the electrochemical results and hydrogen production rate. This work provides an effective strategy to improve the selectivity of Cu-based electrocatalyst and builds a relationship between the adsorption capacity and the electrocatalytic performance. -
![A Double Crown Hexakis[(Di-µ-benzylthio) Nickel] Cluster: Synthesis, Structure and Properties 2011-3309](/Site/default/Uploads/20220711/qq.png "A Double Crown Hexakis[(Di-µ-benzylthio) Nickel] Cluster: Synthesis, Structure and Properties 2011-3309")
ArticleA Double Crown Hexakis[(Di-µ-benzylthio) Nickel] Cluster: Synthesis, Structure and PropertiesLIU E*, JIA Ai-Quan, ZHANG Qian-Feng* and JIAN Fang-Fang
Chin. J. Struct. Chem. 2022, 41, 2203040-2203046 DOI: 10.14102/j.cnki.0254-5861.2011-3309
March 15, 2022
benzylthiol, nickel cluster, porous materials, cyclic voltammetry, thermogravimetry
ABSTRACT
The double crown hexakis[(di-µ-benzylthio) nickel] cluster, [Ni6(SCH2C6H5)12]·C2H5OH, was obtained by reacting C6H5CH2SNa with [(CH3)2CHOCS2]2Ni in EtOH. The results of electrochemical studies show that [Ni6(SCH2C6H5)12] is a quasi-reversible process. The crystal structure of [Ni6(SCH2C6H5)12]·C2H5OH is composed of discrete [Ni6(SCH2C6H5)12] and C2H5OH solvent molecules. Each Ni atom is surrounded by four S atoms of the µ2-SCH2C6H5 ligands in a distorted square-planar structure. The C6H5CH2S- side chains are arranged in the axial and equatorial positions, alternately, concerning the pseudo-hexagonal axis of the molecule. Strong π-π and C–H···π effects form the supramolecular nano-channel along the a-axis in the crystal, which wraps the solvent ethanol molecules in it. In addition, a wall is formed along the b- and c-axes, so that the ethanol molecules can freely enter and leave along the a-axis. These effects result in the ability of the title compound to adsorb and desorb ethanol molecules. Thermogravimetric analysis and powder X-ray diffraction at different temperature are provided to demonstrate this point. -
LetterPreparation, Crystal Structure and Fungicidal Activity of N-(5-(benzofuranol-7-oxymethyl)-1,3,4-thiadiazol-2-yl)amide CompoundsWANG Chun-Nong, ZENG Tai-Ning, LI Sheng-Nan, LI Wan*, LI Long-Fei, CAO Fei and YANG Zi-Hui
Chin. J. Struct. Chem. 2022, 41, 2203211-2203217 DOI: 10.14102/j.cnki.0254-5861.2011-3326
March 15, 2022
N-(5-(benzofuranol-7-oxymethyl)-1,3,4-thiadiazol-2-yl)amide, preparation, crystal structure, antifungal activity
ABSTRACT
A variety of new N-(5-(benzofuranol-7-oxymethyl)-1,3,4-thiadiazol-2-yl)amide compounds (8a-i) were synthesized through four steps from benzofuranol as raw materials. The crystal structure of compound 8a (C17H21N3O3S, Mr = 347.43) was measured by X-ray diffraction, which was classified as monoclinic system, Z = 4, V = 1742.72(8) Å3, Dc = 1.324 Mg/m3, F(000) = 736, S = 1.03, μ = 0.21 mm-1, space group P21 with a = 9.9177(3), b = 8.9519(2), c = 19.8679(5) Å, the final R = 0.035 and wR = 0.105 for 3873 observed reflections (I > 2σ(I)). The X-ray structure presented N(3)–H(3)···N(2) and C(6)–H(6)···O(3) intermolecular hydrogen bonds, which acted as an important role in stabilizing the crystal structure. Additionally, preliminary biological assay on compound 8a showed good fungicidal activity in vivo, with the inhibition of 75% against Pseudoperonospora cubensis at 200 mg/L. -
![Manganese(II) and Copper(I) Compounds Based on Two Derivatives of Imidazo[1,5-a]pyridine: Synthesis, Structures, Magnetic Properties, and Catalytic Activity 2011-3296](/Site/default/Uploads/20220711/eee[1].png "Manganese(II) and Copper(I) Compounds Based on Two Derivatives of Imidazo[1,5-a]pyridine: Synthesis, Structures, Magnetic Properties, and Catalytic Activity 2011-3296")
LetterManganese(II) and Copper(I) Compounds Based on Two Derivatives of Imidazo[1,5-a]pyridine: Synthesis, Structures, Magnetic Properties, and Catalytic ActivityZHANG Qian, CUI Yan-Feng, ZHANG Xia-Mei, LI Ya-Hong* and YAO Jin-Lei*
Chin. J. Struct. Chem. 2022, 41, 2203148-2203154 DOI: 10.14102/j.cnki.0254-5861.2011-3296
March 15, 2022
coordination complexes, chain configuration, magnetism, catalysis
ABSTRACT
The utilization of 2,6-bis(imidazo[1,5-a]pyridin-3-yl)pyridine (bipp) and 3-(pyridin-2-yl)imidazo[1, 5-a]pyridine (pip) in the compounds of manganese(II) and copper(I) ions is presented. Two complexes, [Mn(bipp)(SO4)(H2O)]n (1) and [Cu(pip)2]ClO4 (2), were prepared with different characteristics in structure. Compound 1 exhibits a one-dimensional chain topology, and 2 is a homoleptic Cu(I) complex. The dc magnetic susceptibility investigations reveal the antiferromagnetic (AF) MnII···MnII interactions in complex 1. The catalytic activity of compound 2 toward ketalization reactions was studied. Complex 2 exhibits high activity for the ketalization transformations of aliphatic ketones. -
LetterCyano and Isocyano-substituted Tetraphenylethylene with AIE Behavior and Mechanoresponsive BehaviorQing Liu, Shusheng Yue, Zhangqiang Yan, Yongfa Xie* and Hu Cai*
Chin. J. Struct. Chem. 2022, 41, 2204075-2204082 DOI: 10.14102/j.cnki.0254-5861.2021-0049
April 8, 2022
cyano-group, isocyano-group, tetraphenylethlene (TPE), aggregation induced emission (AIE), mechanochromic
ABSTRACT
Dual-functional materials with AIE behavior and mechanoresponsive behavior have attracted considerable attention due to their promising applications in mechano-sensors, optical storage, solid-state optoelectric devices and bioimage systems. AIEgens bearing tetraphenylethylene (TPE) core become elementary building blocks in many fluorescent functional materials. In this article, cyano and isocyano-electronic withdrawing groups are incorporated with TPE skeleton to form tetracyanophenylethylene (TPE-CN) and tetraisocyanophenylethylene (TPE-NC). Their structures are confirmed by NMR, Mass Spectra and single crystal X-ray measurement. These two isomers reflect aggregation-induced emission (AIE) property in solution state and mechanochromic behavior in solid state. Interestingly, their luminescent intensities, quantum yields and fluorescent lifetime in solid state have an obvious increase upon grinding. The theoretical calculation of these two compounds clarify their difference in optical properties. The mechanochromic mechanism is also intensively explained by powder X-ray measurements. -
CommunicationStrong High Entropy Alloy-Support Interaction Enables Efficient Electrocatalytic Water Splitting at High Current DensityHongdong Li, Yue Pan, Jianping Lai*, Lei Wang* and Shouhua Feng
Chin. J. Struct. Chem. 2022, 41, 2208003-2208011 DOI: 10.14102/j.cnki.0254-5861.2022-0125
July 25, 2022
high entropy alloy, metal-support interactions, microwave heating, water splitting, activity and durability
ABSTRACT
In electrocatalysis, the stability issue between catalyst and support still needs great attention. Here, a series of high- entropy alloy nanoparticles (HEA-NPs) embedded in carbon cloth (CC) were synthesized by using the scalable strategy-microwave heating. Among them, PtRhCoNiCu/CC exhibits outstanding hydrogen evolution reaction (HER) activity (19 and 170 mV overpotential at 10 and 1000 mA cm-2) and stability (150 h), outperforming other recently reported HEAs catalysts. IrRuCoNiCu/CC displays superior oxygen evolution reaction (OER) activity (166 and 354 mV overpotential at 10 and 1000 mA cm-2) and stability (150 h), and shows a lower overpotential than recently reported HEA catalysts. In water splitting, IrRuCoNiCu/CC(+)//PtRhCoNiCu/CC(-) electrolyzer achieves 500 mA cm-2 (1000 mA cm-2) high current density at 1.76 V (1.88 V) and exhibits excellent stability, which is one of the best catalysts currently. Therefore, the novel supported HEA catalyst with high stability is expected to be a promising candidate material for industrialized water splitting. -
CommunicationAn In-Situ Variable-Temperature Surface-Enhanced Raman Spectroscopic Study of the Plasmon-Mediated Selective Oxidation of p-AminothiophenolWumei Cao, Yang Lu and Yi-Fan Huang*
Chin. J. Struct. Chem. 2022, 41, 2210077-2210081 DOI: 10.14102/j.cnki.0254-5861.2022-0134
October 25, 2022
surface-enhanced Raman spectroscopy, p-aminothiophenol, temperature, plasmon-mediated chemical reaction
ABSTRACT
The roles of temperature change in surface-enhanced Raman scattering (SERS) hotspots are important for understanding the plasmon-mediated selective oxidation of p-aminothiophenol in a SERS measurement. Here, we demonstrate that the temperature change in hotspots seriously influences the conversion of p-aminothiophenol on Au by employing variable-temperature SERS measurements. The conversion steadily and irreversibly increased when the temperature increased from 100 to 360 K. But the conversion decreased above 360 K, because this conversion was exothermic. This temperature-dependence conversion suggests that the temperature change in hotspots originated from the photothermal effect should be coupled to the hot-electron effect in promoting the selective oxidation of p-aminothiophenol. -
ArticleBoosting Stable and Fast Potassium Storage of Iron Sulfide through Rational Yolk-Shell Design and Ni Doping
Yanmei Gan, Jiajie Zhu, Qixin Zhang, Chaoying Wang, Lunhui Guan and Yi Zhao*
Chin. J. Struct. Chem. 2022, 41, 2205030-2205036 DOI: 10.14102/j.cnki.0254-5861.2022-0044
May 20, 2022
FeS2, Ni-doping, yolk-shell structure, anode, potassium-ion batteries
ABSTRACT
Metal sulfides have been regarded as promising anodes for potassium-ion batteries (PIBs) due to their high theoretical capacities, while the performance is limited by their intrinsic poor conductivity and large volume fluctuation during the insertion/extraction of large potassium ion. Herein, the battery performance of iron sulfide anode is significantly enhanced through yolk-shell (Y-S) structure design and nickel doping, aiming to realize good structure stability and superior electron/ion transportation. For potassium storage, as-prepared Y-S Ni-FeS2@C shows excellent cyclic performance and sustains high capacities of 328 mA h g-1 after 100 cycles at 0.2 A g-1 and 226 mA h g-1 after 1000 cycles at 1 A g-1. Especially, it displays a superior rate capacity of 200 mA h g-1 at 20 A g-1, higher than that of Y-S FeS2@C and most as-reported metal sulfide anodes for PIBs. The experimental analysis and theoretical calculation illuminate the effect of Ni-doping on decreasing the particle size of iron sulfide and enhancing the ion/electron transport ability, thus accounting for the exceptional rate capability of Y-S Ni-FeS2@C composite. -
ArticleHighly Efficient Photocatalytic CO2 Methanation over Ru-Doped TiO2 with Tunable Oxygen Vacancies
Zheyue Li†, Di Wu†, Wanbing Gong*, Jiayi Li, Shuaikang Sang, Hengjie Liu, Ran Long and Yujie Xiong*
Chin. J. Struct. Chem. 2022, 41, 2212043-2212050 DOI: 10.14102/j.cnki.0254-5861.2022-0212
December 2, 2022
photocatalysis, CO2 methanation, metal doping, titanium oxide, oxygen vacancies
ABSTRACT
Solar-driven CO2 methanation is an imperative and promising approach to relieve the global warming and environmental crisis, yet remains a great challenge due to the low reaction efficiency, unsatisfactory selectivity and poor stability. In this work, we demonstrate a facile and efficient strategy to prepare Ru-doped TiO2 photocatalyst with tunable oxygen vacancies using the ascorbic acid as a reducing agent for the CO2 methanation reaction. The optimal Ru-TiO2-OV-50 exhibits a remarkable CH4 production rate of 81.7 mmol g-1 h-1 with a 100% CH4 selectivity under a 1.5 W cm-2 light illumination, which is significantly higher than commercial Ru/TiO2 and other reported catalysts. We reveal that the superior photocatalytic CO2 methanation performance is mainly due to the synergistic effect of Ru doping and TiO2 with tunable oxygen vacancies. Impressively, the light rather than thermal effect is confirmed as the main influencing factor by experimental studies. In addition, in situ spectroscopic technology is performed to investigate the CO2 methanation reaction pathway. This work will open an avenue to design and prepare highly efficient photocatalyst with tunable oxygen vacancies for CO2 conversion and other related applications.
- Address: Fuzhou High & New Technology Industrial Zone, Shangjie, Minhou, Fuzhou, Fujian 350108, China
- Tel: (86)-591-63173769, 63173770
- E-mail: cjsc@fjirsm.ac.cn