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Materials Today Physics · 2022 · IF 11.021

Electrochemical ammonia synthesis via nitrogen reduction reaction on 1T/2H mixed-phase MoSSe catalyst: Theoretical and experimental studies

Mengjie Sun,Chaoqun Ma,Min Ma,Yanjiao Wei,Shihua Dong,Xiaoli Zhang,Jian Tian,Minhua Shao

Electrocatalytic nitrogen reduction (NRR) is regarded as an energy-efficient technology to produce NH 3 . Nevertheless, achieving high NH 3 yield and Faradaic efficiency (FE) under ambient conditions remains a great challenge. Herein, 1T/2H mixed-phase MoS 0·5 Se 1.5 (named 1T/2H MoSSe) nanoflower, as an efficient non-noble metal NRR electrocatalyst, was synthesized by the one-step solvothermal method. 1T/2H MoSSe realizes an excellent NH 3 yield of 32.32 μg h −1 mg cat. −1 at −0.45 V vs. RHE and an outstanding FE of 12.66% at −0.40 V vs. RHE in 0.1 M HCl, which are better than pure MoS 2 (NH 3 yield: 15.16 μg h −1 mg cat. −1 , FE: 0.35%) and MoSe 2 (NH 3 yield: 26.42 μg h −1 mg cat. −1 , FE: 2.75%). Density functional theory (DFT) calculations exhibit that MoSSe catalyst is structurally favorable to the potential-determining step (PDS, *NH–NH 2 → *NH 2 –NH 2 ) and thus shows increased NRR activity and selectivity. A promising tactic for the rational design of economical, efficient, and durable NRR electrocatalysts is proposed in this work.

CAS / MDL: 15060-55-6
研究领域: 材料科学 · 电化学 · 理论计算
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ACS Catalysis · 2021 · IF 13.084

Activating Edge-Mo of 2H-MoS2 via Coordination with Pyridinic N–C for pH-Universal Hydrogen Evolution Electrocatalysis

Jiayi Qin,Cong Xi,Rui Zhang,Tao Liu,Peichao Zou,Deyao Wu,Qianjin Guo,Jing Mao,Huolin Xin,Jing Yang

It is highly desirable to develop all-pH-compatible hydrogen evolution reaction (HER) electrocatalysts that can be used universally in a variety of different electrolyzers and operated in different pH conditions, i.e., acid, alkaline, microbial, chlor-alkali, etc. So far, two-dimensional layered MoS2 and Mo-based carbon materials have been regarded as promising pH-universal HER electrocatalysts. 2H-MoS2 as a naturally occurring and thermodynamically favorable phase, yet still suffers from poor HER activity in neutral and alkaline electrolytes. Herein, a hybrid electrocatalyst, i.e., 2H-MoS2/N-doped mesoporous graphene, rich in interfacial Mo–pyridinic N coordination is fabricated. The optimized hybrid catalyst delivers long-term durability and outstanding HER activity with overpotentials of 110, 145, and 142 mV at 10 mA cm–2 in acidic, alkaline, and phosphate buffered solutions (PBS) media, respectively, outperforming most of the previously reported MoS2-based catalysts. Theoretical and experimental results demonstrate that the interfacial pyridinic N has a higher tendency to bond with Mo atoms than pyrrolic and graphitic N, and the edge-Mo coordinated with pyridinic N could serve as HER active sites. DFT calculations further reveal that Mo–pyridinic N coordination modifies the charge density of edge-Mo, in turn optimizing the hydrogen absorption energy and facilitating water dissociation, and thereby significantly promoting the intrinsic catalytic activity for the pH-universal HER process.

研究领域: 材料科学 · 电化学 · 催化科学
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RUSSIAN JOURNAL OF GENERAL CHEMISTRY · 2024 ·Vol. 94 ·期 9 ·2356-2364 · IF 0.9

Groundbreaking Benzofused Hybrid Drug: Light-Responsive Reversible Absorption and Release in Hydrogel for Treating Kashin–Beck Disease

Feng L.,Yang J.,Wang J.,Meng S.,Yu H.,Han L.,Zhong W.

Light-controlled release technology uses light signals to regulate drug release. It has potential applications in drug delivery, bioimaging, biosensing, and tissue engineering. In this study, we designed and synthesized light-responsive hydrogels to control the absorption and release of antibiotics. We used Fourier-transform infrared (FT-IR) spectroscopy, X-ray crystallography, scanning electron microscopy (SEM), and thermogravimetric (TGA) to investigate the physicochemical properties of the prepared hydrogel. In the ground state, the photosensitizer forms a stable complex with 7,8-dimethoxy-1,3-dihydro-2 H -3-benzazepin-2-one in the hydrogel matrix. Exposure to 365 nm UV light causes the photosensitizer to undergo photoisomerization, converting from trans to cis structure, releasing the drug into the environment. Biological studies showed that 7,8-dimethoxy-1,3-dihydro-2 H -3-benzazepin-2-one released from the hydrogel significantly reduced IL-1β and IL-6 levels in chondrocytes, demonstrating anti-inflammatory effects. This study provides a new approach for developing light-responsive hydrogels for drug delivery applications.

研究领域: 药物递送 · 生物材料 · 炎症研究
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Case Studies in Thermal Engineering · 2024 · IF 6.4

Synthesis of short-chain fluorocarbon surfactant: Enhancing surface and foam performance through hydrocarbon surfactants compounding

Wenjun Zhao,Zhisheng Xu,Long Yan,Guoqing Niu

The research of short-chain fluorocarbon surfactants is crucial in effectively and environmentally extinguishing petrochemical fires. In this study, a short-chain fluorocarbon surfactant named 2 H ,2 H -perfluorooctanoic acid sodium salt (PFH-CA) was synthesized, and then characterized its chemical structure, thermal stability, surface activity, and foam property. Subsequently, PFH-CA was compounded with hydrocarbon surfactants including sodium dodecyl sulfate (SDS), dodecyl trimethyl ammonium chloride (DTAC), and N , N -dimethyldodecylamine- N -oxid (OB-2) at different molar ratios. The surface tension, interaction parameters, and foam property of the PFH-CA/hydrocarbon surfactant compounding systems were investigated. The analysis indicates that PFH-CA exhibits excellent surface activity and thermal stability concomitant with poor foam property. Introducing SDS, DTAC, and OB-2 enhances the foam performance and reduces the consumption of PFH-CA through synergistic interactions. Especially, PFH-CA/DTAC (1:4) system possesses the strongest interactions and the best performance, with critical micelle concentration ( CMC ) and surface tension at CMC ( γ CMC ) of 0.11 mmol/L and 20.90 mN/m, respectively. When concentration of PFH-CA exceeds 0.5 mmol/L, the foaming ability and foam stability stabilize at 30 cm and 90 %, respectively. The enhanced performance of PFH-CA/DTAC system is attributed to the electrostatic attraction between anionic and cationic surfactants, which facilitates the formation of micelles, subsequently leading to better surface activity and foam properties.

CAS / MDL: 141-78-6 647-42-7
研究领域: 化学 · 材料科学 · 消防安全工程
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BMC Chemistry · 2019 ·Vol. 13 ·期 1 ·1-7 · IF 0

Chemical modification of Bombyx mori silk fibers with vinyl groups for thiol-ene click chemistry

Zhang Xiaoning,Liang Jianwei,Chen Zhenyu,Donley Carrie,Liu Yuling,Cheng Guotao

Natural Bombyx mori silk fibroin (SF) fibers were modified with 2-methacryloyloxyethyl isocyanate (MOI) first for the introduction of vinyl groups. Then, 1H,1H,2H,2H-perfluorodecanethiol was grafted onto the SF fibers via thiol-ene click chemistry using ultraviolet light. The formations of MOI-modified and PFDT-grafted SF fibers were analyzed using Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy, respectively. The morphology of samples was also revealed by a scanning electron microscope. In addition, differential scanning calorimetry results demonstrated that SF fibers did not show significant change in thermal behavior, regardless of the chemical modification. To confirm the cytotoxicity of the prepared SF fibers, MTT [3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide] assay was performed, and no toxicity was observed with PFDT-grafted SF fibers. The results also showed that PFDT-grafted SF fibers exhibited good antifouling properties when Chlorella vulgaris (C. vulgaris) was selected as a model for algal cells adhesion experiment.

CAS / MDL: 77-58-7 67-68-5 123-31-9
研究领域: 材料科学 · 表面化学 · 生物医学工程 · 高分子化学
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LANGMUIR · 2020 · IF 3.557

Robust Superamphiphobic Coatings Based on Raspberry-like Hollow SnO2 Composites

Xinting Han,Junyan Peng,Shaohua Jiang,Jian Xiong,Yu Song,Xiao Gong

Good mechanical and chemical stabilities are the key factors for the wide application of superhydrophobic surfaces. In this work, we first prepared raspberry-like hollow structured SnO2 nanoparticles using a simple hydrothermal method, followed by an annealing step. Then, the intrinsic raspberry-like hollow SnO2 nanoparticles were combined with hydrophilic SiO2 nanoparticles to construct rough surfaces with suitable hierarchical structures, and 1H,1H,2H,2H-perfluorodecyltriethoxysilane (FAS-17) was used as a hydrophobic modifier of SnO2, while epoxy resin was used as an adhesive to prepare a superamphiphobic coating with good stability and durability. Such a coating can be applied on various substrates using a simple spray-coating or drop-coating method. The water contact angle and diiodomethane contact angle of the coating could reach up to ∼165 and ∼151°, respectively. After various chemical and mechanical stability tests including hot water treatment, salt water corrosion, strong adhesive tape peeling, and kneading, the coatings still remained amphiphobic. The facile fabrication of the robust superhydrophobic coating has great potential for applications in real life and industrial production.

CAS / MDL: 75-11-6 112945-52-5
研究领域: 材料科学 · 表面化学 · 纳米技术 · 涂层与薄膜
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Synergistic enhancement of hydrogen evolution reaction by one-step pyrolysis synthesis of 1T-2H MoS2 loaded nitrogen-doped carbon

Jiabo Wang,Zhentao Liu,Wenxin Wang,Li Chen

The increasing demand for clean and renewable energy underscores the importance of hydrogen energy, with electrocatalytic water splitting being an efficient method for green hydrogen production. Platinum, while an excellent catalyst for hydrogen evolution reactions (HER), is hindered by high cost and scarcity. This study explores non-precious alternatives, focusing on MoS 2 due to its “platinum-like behavior.” The 1T-2H MoS 2 loaded on N-doped carbon (NC) catalysts (1T-2H MoS 2 @NC) were synthesized through a one-step pyrolysis of melamine and ammonium thiomolybdate. Comprehensive analysis revealed that the 2H phase formed at 700 °C, transitioning to a biphasic 1T-2H composition at higher temperatures. The catalyst synthesized at 800 °C with a 1:8 reactant ratio demonstrated exceptional HER performance, with an overpotential of 175 mV at 10 mA cm −2 and a Tafel slope of 92.37 mV dec −1 . This study highlights the potential of 1T-2H MoS 2 @NC as a cost-effective and efficient catalyst for sustainable hydrogen production.

CAS / MDL: 15060-55-6 108-78-1
研究领域: 材料科学 · 能源化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Dual-vacancies modulation of 1T/2H heterostructured MoS2-CdS nanoflowers via radiolytic radical chemistry for efficient photocatalytic H2 evolution

Chong Chen,Qiuhao Li,Fengqing Wang,Changjiang Hu,Jun Ma

Precise defect engineering of photocatalysts is highly demanding but remains a challenge. Here, we developed a facile and controllable γ-ray radiation strategy to assemble dual-vacancies confined MoS 2 -CdS-γ nanocomposite photocatalyst. We showed the solvated electron induced homogeneous growth of defects-rich CdS nanoparticles, while the symbiotic • OH radicals etched flower-like 1T/2H MoS 2 substrate surfaces. The optimal MoS 2 -CdS-γ exhibited a H 2 evolution rate of up to 37.80 mmol/h/g under visible light irradiation, which was 36.7 times higher than that of bare CdS-γ, and far superior to those synthesized by hydrothermal method. The microscopic characterizations and theoretical calculations revealed the formation of such unprecedented dual-sulfur-vacancies ensured the tight interfacial contact for fast charge separation. Besides, the existence of 1T-MoS 2 phase further improved the conductivity and strengthened the adsorption interaction with H + intermediate. Therefore, the radiolytic radical chemistry offered a facile, ambient and effective synthetic strategy to improve the catalytic performances of photocatalytic materials.

CAS / MDL: 12054-85-2 7772-98-7
研究领域: 材料科学 · 纳米技术 · 光催化 · 化学工程
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY · 2018 ·Vol. 135 ·期 4 ·2317-2328 · IF 2.209

Synthesis and thermal decomposition behavior of nitrogen- and oxygen-rich energetic material N-trinitromethyl-4,5-dicyano-2H-1,2,3-triazole

Yin Xin,Li Jie,Zhang Guojie,Gu Hao,Ma Qing,Wang Shumin,Wang Jun

N -trinitromethyl-4,5-dicyano-2 H -1,2,3-triazole was readily synthesized from 4,5-dicyano-2 H -1,2,3-triazole. Its crystal structure was obtained for the first time and its crystalline density in 296 K was 1.729 g cm −3 . It shows high nitrogen and oxygen content up to 77.6%, high calculated solid heat of formation (564 kJ mol −1 ), and superior detonation pressure and detonation velocity ( D  = 8619 m s −1 , P  = 30.8 GPa). This new hydrogen-absent explosive shows high impact and friction sensitivities ( IS : 1.25 J, FS : 32 N), which is lower than commercial primary explosive 2-diazonium-4,6-dinitrophenol (DDNP) ( IS : 1 J, FS : 5 N). The relationship between intermolecular interaction and sensitivity as well as thermal stability of the title compound was investigated by Hirshfeld surface analysis and fingerprint plot. Its thermodynamic properties were studied by non-isothermal kinetic methods based on the results of differential scanning calorimeter. It is interesting that apparent activation energy ( E a ) at T p1 (210.89–214.17 kJ mol −1 ) is higher than those at T p2 (133.90–134.87 kJ mol −1 ). In addition, gaseous product of this new energetic compound was analyzed by the rapid scanning Fourier transform infrared spectroscopy from 20 to 200 °C and its detonation products was theoretically predicted. Based on the decomposition products, its decomposition mechanism was discussed under inert atmosphere. It is undoubted that these significant physicochemical properties make N -trinitromethyl-4,5-dicyano-2 H -1,2,3-triazole a potential hydrogen-absent primary explosive.

研究领域: 化学 · 材料科学 · 物理化学
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Activating the Basal Plane of 2H-MoS2 by Doping Phosphor for Enhancement in the Photocatalytic Degradation of Organic Contaminants

Yanei Xue,Penghui Shao,Yixing Yuan,Wenxin Shi,Fuyi Cui

The 2H phases of MoS2 (2H-MoS2) monolayers present a wealth of new opportunities in photocatalysis owing to their photoinduced catalyzing ability and excellent charge carrier mobility. However, the complete release of their catalytic activities is restricted by their inert basal planes. Although the inert base planes of 2H-MoS2 are known to be activated by atomic doping, the operational principle of the exotic atoms remains vague. In this study, the unutilized inert base sites of MoS2 were activated via an oxygen-aided P-substituted method (denoted as POMS). Molecular structural tests and analyses of POMS indicated that the inert MoS2 substrate is activated when the inerratic crystal phases transform to amorphous phases in the P-doping process. The fully activated inert base planes provide sufficient reaction sites for photo-oxidized water contaminants. The designed POMS presented superior activity in organic degradation and completely removed sulfamethoxazole within 20 min. Uncovering these operational principles provides a theoretical basis for designing effective catalysts.

研究领域: 材料科学 · 环境科学
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DESALINATION · 2022 · IF 11.211

1T/2H MoS2 nanoflowers embedded in porous PDMS sponge with high salt-resistance for efficient and durable solar desalination

Jing Jiang,Huiling Jiang,Ying Xu,Lunhong Ai

Solar water evaporation is emerging as one of the most cost-effective and sustainable technologies for efficient seawater desalination . However, salt crystallization during solar desalination severely limits light absorption and reduces evaporation efficiency. Balancing the desirable evaporation rate and the suppressed salt crystallization is critical for long-term solar desalination, but remains a major challenge. In this work, 1T/2H MoS 2 nanoflower embedded in a macroporous PDMS sponge (MoS 2 /PDMS) was fabricated and used as a novel solar evaporator for efficient and durable solar desalination. Thanks to the broadband absorption of MoS 2 and the thermal insulating PDMS sponge, the MoS 2 /PDMS sponge presents a high evaporation rate of 1.47 kg m −2  h −1 and an evaporation efficiency of 81.5 % in pure water under one sun irradiation (1 kW m −2 ). Importantly, the MoS 2 /PDMS sponge with macroporous structure and wet-state hydrophilic wettability achieves efficient and durable solar desalination in simulated seawater (3.5 wt% NaCl solution), effectively suppressing salt crystallization. This finding offers a new way to design robust evaporators with structural flexibility, efficient evaporation and durable desalting for solar desalination.

研究领域: 材料科学 · 环境科学
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

1T/2H MoS2 nanoflowers decorated amorphous Mo-CoSx skeleton: A ZIF-based composite electrocatalyst for the hydrogen evolution reaction

Chencheng Gao,Hongfeng Hua,Ming Du,Jinsong Liu,Xiaoyu Wu,Yong Pu,Xing'ao Li

Electronic regulation through component precise control at the atomic level of electrocatalysts has a fundamental influence on the efficiency of hydrogen evolution reaction (HER). Herein, we successfully demonstrate a ZIF-based charge transfer medium for improving the electrocatalytic activity of MoS 2 towards HER. Benefit for the enough porous structure, superior electron conductivity as well as the synergistic effect from the doped atoms, the hybrids phase (1T/2H) MoS 2 nanoflowers decorated amorphous Mo-CoS x skeleton exhibited the promotional electrocatalytic performance in efficiency and stability. Specifically, an extremely low overpotential of 73 mV at the current density of −10 mA cm −2 and an impressive Tafel slope of 39.2 mV dec −1 had been achieved from the nanocomposites in an acidic condition (0.5 M H 2 SO 4 ). The satisfactory activity improvement can be ascribed to the enhancement of electronic transmission rate as well as the synergistic effects between the doped Mo element and CoS x . This work might develop a new avenue to design highly efficient multicomponent electrocatalysts towards HER.

研究领域: 材料科学 · 电化学
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