MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Yu Zhou,Hui Gong,Hou-Jing Liu
Efficient, selective and highly sensitive detection of H 2 S is important for environmental protection and human security. Nanomaterials-based cataluminescence (CTL) sensors, especially metal-free catalysts, have been used for gas sensing. Herein, due to the efficient electron transfer and high specific area of silicon nitride (Si 3 N 4 ), combined with the strong electronegativity of fluorine and oxygen, we purposely synthesized F and O-modified Si 3 N 4 (F/O-Si 3 N 4 ) by engineering surface states and catalytic properties. We then used it to construct a H 2 S CTL gas sensor. Compared with other metal-based CTL sensors, the F/O-Si 3 N 4 -based CTL system exhibited high sensitivity and a longer lifetime stability. The detection limit was 0.027 μg mL −1 in the detection range of 0.49–8.17 μg mL −1 , and a relative standard deviation (RSD) of better than 3.3% were obtained. Further research demonstrated the luminescence mechanism, in which the rich oxygen vacancies of Si 3 N 4 promoted the adsorption of O 2 and the formation of F-Si sites due to the catalytic oxidation of H 2 S and the generation of SO 2 *. This served as the main emitter accounting for the strong CTL emission. This work is the first report of the application of Si 3 N 4 as a catalyst for CTL H 2 S sensing. This will expand the methods for enhancing the catalytic activity and practical applications of metal-free materials.
研究领域:
材料科学
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环境科学
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传感器技术
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Guiming Ba,Zhiwei Liang,Haiping Li,Na Du,Jianqiang Liu,Wanguo Hou
Graphite carbon nitride (CN) is considered as a promising photocatalyst for solving current energy and environmental crises, but its practical application is still restricted by fast recombination of photogenerated charge carriers, low specific surface area, and narrow visible light absorption range. Herein, oxygen-modified CN (MCN) with simultaneous formation of massive mesopores and homojunctions was successfully synthesized by calcining the precursor, a cyanuric acid (CYA)-loaded melamine (MA) hierarchical structure composed of nanobelts, which was prepared for the first time. MCN exhibits accelerated charge separation, increased specific surface areas, and enhanced visible light absorption, compared with CN, and these jointly render the photocatalytic hydrogen evolution rate of MCN (934 μmol h −1 g −1 ) be about five times higher than that of CN (163 μmol h −1 g −1 ). MCN also exhibits much faster singlet oxygen generation and higher photoactivity in organic degradation. The MA hierarchical structure and CYA synergistically formed the new mesopores and C O C bonds in MCN, which cause prominent upper shift of the Fermi level and enhanced photoabsorption of MCN. Besides, electronic microscopy images distinctly show two different sorts of regions in MCN, i.e. those with massive and few mesopores (marked as MPCN and NPCN), respectively. Therefore, MPCN/NPCN homojunctions were probably constructed in MCN, which leads to the accelerated charge separation. This work gives a way to form simultaneously mesopores and homojunctions in CN and illustrates the formation mechanism, which can effectively direct synthesis of similar photocatalysts.
研究领域:
材料科学
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环境科学
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能源科学
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DOI
高影响因子
Advanced Materials Interfaces
·
2020
·Vol. 7
·期 7
·1901933
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IF 4.948
Qianfang Tang,Min Zhong,Hao Liu,Xiangying Chen,Zhongjie Zhang,Shuanghong Chen
In present work, commercial microporous carbon materials are modified on the surface with phosphorus/oxygen species by using phytic acid as sole dopant, which plays crucial effect on the carbon structure, wettability, electrical conductivity, and capacitive behaviors. It reveals that with increasing the content of heteroatoms, the porosity and contact angle are decreased but the conductivity turns much larger. Furthermore, p- aminophenol is introduced to serve as redox additive, which can produce more active surface sites by forming hydrogen bond and complexation with the surface functional groups, further providing additional pseudo-capacitance. As a result, the energy density of carbon sample by phosphorus/oxygen doping in 1 m H 2 SO 4 electrolyte with p- aminophenol is as high as 9.2 Wh kg −1 , which is 2.6 than that of pristine carbon. What is more, in terms of the simple operation and effective performance, the integration of surface modification toward carbon materials and redox additive can be favorable for largely enhancing the supercapacitor performance.
研究领域:
材料科学
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电化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yanqing Cong,Shiyi Zhang,Qiuang Zheng,Xinyue Li,Yi Zhang,Shi-Wen Lv
Photocatalytic oxygen reduction is regarded as the cleanest approach for the production of hydrogen peroxide (H 2 O 2 ). Herein, oxygen-modified graphite carbon nitride (g-C 3 N 4 ) with nitrogen-defect (namely g-C 3 N 4 -ND4-OM3) was synthesized by a feasible method. Owing to the existence of nitrogen vacancy and oxygen-containing functional group, the absorption bands derived from n → π* and π → π* electronic transitions were enhanced, thereby enlarging the visible light response range of catalysts. Interestingly, nitrogen-defect can capture electron and effectively suppress the recombination of photoinduced electrons and holes. More importantly, the introduction of oxygen-containing functional groups can improve the hydrophilicity of g-C 3 N 4 , which was beneficial for the adsorption of dissolved oxygen. The electrostatic potential distributions of g-C 3 N 4 -based photocatalyst structural unit were also changed after introducing nitrogen vacancy and oxygen-containing functional group, and the electron-donating ability of g-C 3 N 4 was improved. As a result, the evolution rate of H 2 O 2 catalyzed by g-C 3 N 4 -ND4-OM3 was as high as 146.96 μmol/g/L under visible light irradiation. The photocatalytic H 2 O 2 generation was completed through the direct 2-e − oxygen reduction. In short, current work will share novel insights into photocatalytic H 2 O 2 generation over g-C 3 N 4 -based catalyst.
研究领域:
材料科学
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环境科学
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化学
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DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2024
·Vol. 31
·期 11
·16940-16957
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IF 0
Lyu Shiqi,Abidin Zurina Zainal,Yaw Thomas Choong Shean,Resul Mohamad Faiz Mukhtar Gunam
The applications of polysulfides derived from natural plant oil and sulfur via the inverse vulcanization in the removal of heavy metals from aqueous solutions suffered from their low porosity and scarce surface functionality because of their hydrophobic surfaces and bulk characteristics. In this study, polysulfides from sulfur and palm oil (PSPs) with significantly enhanced porosity (13.7–24.1 m 2 /g) and surface oxygen-containing functional groups (6.9–8.6 wt.%) were synthesized with the optimization of process conditions including reaction time, temperature, and mass ratios of sulfur/palm oil/NaCl/sodium citrate. PSPs were applied as sorbents to remove heavy metals present in aqueous solutions. The integration of porosity and oxygen modification allowed a fast kinetic (4.0 h) and enhanced maximum sorption capacities for Pb(II) (218.5 mg/g), Cu(II) (74.8 mg/g), and Cr(III) (68.4 mg/g) at pH 5.0 and T 298 K comparing with polysulfides made without NaCl/sodium citrate. The sorption behaviors of Pb(II), Cu(II), and Cr(III) on PSPs were highly dependent on the solution pH values and ionic strength. The sorption presented excellent anti-interference capability for the coexisting cations and anions. The sorption processes were endothermic and spontaneous. This work would guide the preparation of porous polysulfides with surface modification as efficient sorbents to remediate heavy metals from aqueous solutions.
研究领域:
环境科学
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材料科学
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DOI
PubMed
LIQUID CRYSTALS
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2019
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IF 3.078
Shengbo Zhu,Yangyang Zhu,Jin Chigan,Yuqiao Fu,Qiang Weng,Xiaoling Niu,Weixing Chen,Ran Chen,Xinbing Chen,Zhongwei An
A series of biphenyl ester compounds with alkenyl, alkyl, oxirane, and 1,3-dioxolane as the terminal groups have been synthesised for investigating the mesomorphic and thermal stability. Based on the same carbon skeleton, the allyl-terminated compound V1OLC has no mesophase, while the oxirane-terminated compound POLC not only has wider multiple smectic mesophase compared with the propyl-terminated compound 3OLC but also exhibits the best thermal stability. However, when the terminal groups change from oxirane to 1,3-dioxolane, EOLC shows neither mesophase nor the good thermal stability. In addition, with the extension of the terminal chains, the butyl-terminated compound 4OLC gives the widest smectic mesophase. These imply that the mesomorphic and thermal stability of these biphenyl ester compounds are dependent on the suitable terminal chain lengths and epoxy sizes. Meanwhile, Density Functional Theory (DFT) calculations were conducted to assist in analysing the experimental results.
研究领域:
材料科学
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物理化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Xuecheng Cao,Minghui Cui,Kaiqi Fang,Liting Yan,Hongyu Gong,Yu Zhang,Xiangjun Zheng,Ruizhi Yang
Rechargeable non-aqueous lithium-oxygen batteries (LOBs) have garnered increasing attention owing to their high theoretical energy density. However, their slow cathodic kinetics hinder efficient battery reactions. Nanoscale catalysts can effectively enhance electrocatalytic activity and atomic utilization efficiency. However, the agglomeration of nanoscale catalysts (such as cluster and single atoms) during continuous discharge/charge cycles leads to decreased electrochemical performance and poor cyclic stability. Herein, the ruthenium (Ru) atomic sites anchored on an O-doped molybdenum disulfide (O-MoS 2 ) catalyst (designated as Ru/O-MoS 2 ) was fabricated using a facile impregnation and calcination method. Strong Ru-O coupling between Ru atoms and the O-MoS 2 substrate optimizes the localized electronic structure, resulting in improved electrochemical performance and enhanced resistance to Ostwald ripening. When employed as a cathode catalyst for LOBs, Ru/O-MoS 2 catalyst exhibits a high reversible specific capacity (18700.5 (±59.8) mAh g −1 ), good rate capability, and enhanced long-term stability (115 cycles, 1200 h). This study encourages facile and efficient strategies for the development of effective and stable electrocatalysts for use in LOBs.
研究领域:
材料科学
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电化学
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DOI
高影响因子
ACS Catalysis
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2024
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IF 11.3
Yang Zhang,Ning Cao,Xiaoming Liu,Fengting He,Yangming Lu,Shuling Wang,Chaocheng Zhao,Yongqiang Wang,Jinqiang Zhang,Shaobin Wang
Photocatalytic seawater splitting to produce clean hydrogen from nonpotable water using sunlight is a crucial endeavor. However, the scarcity of high-performance photocatalysts in the promising yet fledgling field presents a formidable challenge. Herein, we successfully synthesized a crystalline oxygen-modified carbon nitride (CCNO) polymeric semiconductor that served as an effective photocatalyst for seawater splitting. Comprehensive characterizations and theoretical calculations revealed that nitrogen vacancies and bridging oxygen in the CCNO lattice acted as potent Lewis acid–base pairs, creating an enhanced built-in electric field. This advancement significantly accelerated charge dynamics and bolstered resistance to ionic interference in seawater. Consequently, CCNO exhibited a robust photocatalytic H2 evolution activity of 29.51 mmol g–1 h–1 in natural seawater, with an impressive apparent quantum efficiency of 66.86% under 420 nm monochromatic light. Seawater splitting for H2 production reached 16.83 mmol g–1 under natural light irradiation for 3 h (9–12 o’clock), showcasing its great potential for practical applications. This work presents strategies for developing a metal-free photocatalyst and elucidates its reaction mechanism in the seawater splitting process, laying the foundation for scalable production of clean hydrogen.
研究领域:
材料科学
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能源化学
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环境科学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2025
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IF 9.5
Youpeng Cao,Hongling Liu,Yuxuan Xiao,Lun Li,Jiao Yang,Chunfa Liu,Chengcheng Zhong,Wendi Zhang,Shuyang Peng,Junge Yang,Zhichao Yu,Weng Fai Ip,Hui Pan
Platinum (Pt) is a highly efficient catalyst for the hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR). However, the scarcity of Pt necessitates the development of catalysts with low Pt content while maintaining high activity. In this study, we report the synthesis of oxygen-modified supra-nanometer-sized RuPt nanocrystals with low Pt content by a simple air annealing method to achieve a catalyst with high activity. The annealed catalyst, RuPt/C-200, exhibits a very low overpotential of only 3.8 mV at 10 mA cm−2, a low Tafel slope of 16.6 mV dec−1, and a 2.8-fold increase in mass activity at an overpotential of 0.06 V for HER compared to the unannealed catalyst. Additionally, the HOR exchange current density increases 2.9-fold compared to the unannealed catalyst. AEMWE tests confirm the application potential of RuPt/C-200, while density-functional-theory (DFT) calculations reveal that oxygen modification, by optimizing the hydrogen binding energy, plays a crucial role in improving the catalytic performance of RuPt. This work highlights that combining the oxygen modification strategy with the nanoscale size effect could advance the development of high-performance RuPt electrocatalyst for both alkaline HER and HOR.
研究领域:
材料科学
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电化学
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理论计算
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产品关联
DOI
高影响因子
Journal of Magnesium and Alloys
·
2025
·
IF 13.8
Fanfan Liu,Xiaomeng Fan,Xinyue Gao,Jinjin Ban,Guoqin Cao,Shilin Zhang,Junhua Hu
Rechargeable Mg/Li hybrid ion batteries with Mg 2+ /Li + double-salt electrolytes and safe Mg anodes are a viable option for large-scale energy storage. Nevertheless, achieving the desired reasonable electrochemical performance remains a great challenge due to the capacity limitations of conventional Li-intercalation cathodes. To mitigate this limitation, the 3D oxygenated MXene Ti 3 C 2 @CoS 2 /FeS 2 (denoted as o-Ti 3 C 2 @CoS 2 , o-Ti 3 C 2 @FeS 2 ) with both dual-storage mechanism and multidimensional structure to achieve the desirable storage capacity is engineered. Benefiting from the formation of special structure and interfacial chemical bonds Ti–O–Co/Ti–O–Fe, as well as the electronegative o-Ti 3 C 2 weaken the Co–S/Fe–S bonds, the o-Ti 3 C 2 @CoS 2 cathode exhibits superior capacity up to 425 mAh g −1 at 100 mA g −1 and overwhelming advantageous ultra-long life over 2,400 cycles at 500 mA g −1 . Simultaneously, the o-Ti 3 C 2 @FeS 2 also displays a high-rate capability, outstanding cycling stability, and fast diffusion kinetics. Furthermore, the conversion reaction of Mg 2+ /Li + co-intercalation and the charge storage mechanism during cycling are thoroughly clarified by systematic ex-situ characterizations and theoretical computations. This study reveals the influence of MXene electrode structure on the importance of electrochemical performance and provides guidance for the future design of high-performance MXene materials for energy storage applications.
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高影响因子
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