NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 49
·期 1
·132-140
·
IF 2.7
Rumeng Feng,Lu Chen,Liping Huang,Haihong Wu,Yuanyu Ge,Jiani Xu,Min Zeng,Wenyao Li
The synergistic effect between the transition metal sulfide alloy core, the N-doped graphene shell, and the internal interfacial potential serves to regulate the electronic structure and facilitate electron transfer. We used Fe-based Prussian blue analogues as a single precursor to prepare a N-doped graphene-coated metal core–shell structure (FeNi@NG) through hydrothermal and high-temperature solid phase reactions. The S source was then introduced and annealed, yielding a S, N co-doped graphene-encapsulated metal core–shell structure (FeNi–S@NG). Finally, a nitrogen-doped graphene-coated metal core–shell structure with S defects (S–FeNi@NG) was obtained through NaBH4 liquid-phase reduction. The synergistic effect between the transition metal sulfide alloy core and the N-doped graphene shell, in conjunction with the internal interfacial potential regulate the electronic structure and facilitate electron transfer. Numerous sulfur vacancies accelerate electron transfer and enhance OER catalytic performance. The optimized material, S–FeNi@NG, exhibited excellent OER catalytic performance, with an overpotential of 250 mV (at 10 mA cm−2) and a Tafel slope of 90.95 mV dec−1 in an alkaline electrolyte.
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RSC Advances
·
2016
·Vol. 6
·期 90
·87461-87468
·
IF 3.289
Qing Ge,Dingshuo Lou,Shui Lu,Wei Zhang,Li Zhang,Xinping Wang
Poly(ionic liquid)s (PILs) have promising potential to form assemblies with ordered structures in organic media, but experimental investigation on the detailed aggregation behavior of PILs has seldom been involved. In this study, a series of N-alkyl imidazolium-based PILs with different chemical composition in their n-propanol solution was investigated by conductivity measurements. TEM images indicate that PILs with long alkyl chains exhibit onion-like multilamellar structures. The thermodynamic parameters suggest that aggregation of PILs in their good solvents (n-PrOH) is spontaneous, driven by entropy change associated with a hydrophobic effect. As increasing alkyl chain length from 8 to 16, the contribution of per alkyl chain to ΔGθm for PIL aggregation is found to decrease by more than 2 times. The nonsolvent (H2O) contribution to change of Gibbs free energy as well as critical aggregation concentration (CAC) decrease linearly with the volume fraction of water in mixed solvents, implying that PIL aggregation becomes more favorable with the addition of nonsolvent. The results mentioned above play an important role in understanding the aggregation process of PIL in an organic solvent and developing functional materials with well-ordered structures.
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CRYSTENGCOMM
·
2019
·Vol. 21
·期 40
·6010-6017
·
IF 3.382
Shuai Fang,Hongan Ma,Zhanke Wang,Zhiqiang Yang,Zheng-hao Cai,Luyao Ding,Xinyuan Miao,Liangchao Chen,XiaoPeng Jia
FeS is the main sulfur-containing compound in natural diamond inclusions. The research on FeS-doped diamond crystals plays an extremely important role in exploring the growth environment of natural diamond and the chemical composition of the earth. In our work, the characteristics of FeS doped diamond crystals were studied by using a China-type large volume cubic high-pressure apparatus with an iron–nickel alloy as a catalyst at 6.0 GPa and 1300–1350 °C. The crystals were characterized by OM, SEM, XPS, FTIR and Raman. Scanning electron microscopy of the crystal shows that the {100} plane of the crystal is rougher than {111}, which is related to the number of dangling bonds on different crystal faces of the crystal. The residue on the surface of the crystal was detected by mapping, and the test result showed that it was a sulfur iron and a sulfur nickel compound. FeS will decompose in the synthesis system, and the decomposition products are Fe and S2.The XPS spectrum of the crystal shows that S was successfully incorporated into the diamond lattice by forming C–S–O and C–S–SO2–C bonds, and the peak intensity was strong. The infrared spectrum shows that the N content in the crystal gradually increases as the doping ratio increases. Raman spectroscopy analysis shows that the S-doped Ib-type diamond single crystal has a high-quality sp3 structure, and the full width at half maximum (FWHM) of the crystal gradually broadens as the doping ratio increases.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Ning Li,Wenwen Zhao,Linping Li,Yangqin Gao,Lei Ge
Photocatalysts with hollow structures have drawn great interest owing to their high specific surface area, which can enhance the photocatalytic performance. Herein, we designed the hollow cubic Cu2–xS@Ni–Mo–S nanocomposites by vulcanizing from the Cu2O template and loading the Ni–Mo–S lamellas. The Cu2–xS@Ni–Mo–S composites greatly improved the photocatalytic hydrogen performance. Among them, Cu2–xS–NiMo-5 achieved the optimal photocatalytic rate of 1326.07 μmol/g h, which is approximately 3.85 times higher than that of hollow Cu2–xS (344 μmol/g h) and had good stability for 16 h. The enhanced photocatalytic property was attributed to the metallic behavior of bimetallic Ni–Mo–S lamellas and the LSPR (localized surface plasmon resonance) effect of Cu2–xS. The bimetallic Ni–Mo–S can effectively capture the photogenerated electrons and quickly transfer-diffuse to produce H2. Meanwhile, the hollow Cu2–xS not only provided many more active sites to take part in the reaction but also introduced the LSPR effect to increase the solar utilization. This work provides valuable insights into the synergistic effect of using non-precious metal co-catalysts and the LSPR materials to assist in the photocatalytic hydrogen evolution.
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Scientific Reports
·
2016
·Vol. 6
·期 1
·1-8
·
IF 5.228
He Na,Zhong Lei,Xiao Min,Wang Shuanjin,Han Dongmei,Meng Yuezhong
Sulfur is a promising cathode material with a high theoretical capacity of 1672 mAh g −1 , however, the practical energy density of Li-S battery is far away from such promising due to its low active material utilization and low sulfur loading. Moreover, the challenges of the low electrical conductivity of sulfur and the high solubility of polysulfide intermediates still hinder its practical application. Here, we report a kind of free-standing and foldable cathodes consisting of 3D activated carbon fiber matrix and sulfur cathode. The 3D activated carbon fiber matrix (ACFC) has continuous conductive framework and sufficient internal space to provide a long-distance and continuous high-speed electron pathway. It also gives a very larger internal space and tortuous cathode region to ACFC accommodate a highly sulfur loading and keeps polysulfide within the cathode. The unique structured 3D foldable sulfur cathode using a foldable ACFC as matrix delivers a reversible capacity of about 979 mAh g −1 at 0.2C, a capacity retention of 98% after 100 cycles, and 0.02% capacity attenuation per cycle. Even at an areal capacity of 6 mAh cm −2 , which is 2 times higher than the values of Li-ion battery, it still maintains an excellent rate capability and cycling performance.
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LANGMUIR
·
2025
·
IF 3.9
Chenxiang Feng,Wei Jian,Junxiu Chen,Agula Bao
The environmental problems caused by excessive CO2 emissions have made the development of adsorbent materials for capturing CO2 an important topic. N-doped porous carbon materials are attractive for CO2 adsorption because of their large specific surface area, porous structure, and multiple active sites. S and N are known to work well together as codopants, but the effects of S on N and the synergistic effects of S and N on carbon materials need to be clarified. In this study, N and S codoped porous carbon samples with an ultramicroporous structure were prepared by using lignin as the carbon source and thiourea as the sulfur source. The prepared samples had a specific surface area of up to 1723 m2/g and N and S contents of up to 1.60 at % and 0.23 at %, respectively. In tests, the best-performing sample had a CO2 adsorption capacity of 3.58 mmol/g at 298 K and 1 bar, which can be attributed to ultramicropores (<1 nm) making up 67.8% of the pore volume. S doping had the synergistic effect of increasing the pyrrole N content on the sample surface, which increased the CO2 adsorption capacity. The present study provides insights into using N and S codoping to develop high-efficiency carbon-based adsorbents for CO2 capture.
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CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Jiafa Chen,Peng Bai,Shibo Yuan,Yi He,Zifan Niu,Yicheng Zhao,Yongdan Li
Designing highly efficient photocatalyst for the valorization of CO 2 is an ideal strategy to reduce greenhouse gas emissions and utilize solar energy. In this study, a S-scheme heterojunction photocatalyst is fabricated by solvothermal impregnation of ZnO on W 18 O 49 for photocatalytic CO 2 N -formylation of aniline. The localized surface plasmon resonance effect of W 18 O 49 improves the absorption capacity for long-wave light significantly, and the hot electrons generated in W 18 O 49 with a high energy can migrate to the conduction band of ZnO and thus enhance the photocatalytic reduction ability. Meanwhile, the S-scheme heterojunction facilitates the separation of photoinduced charge carriers and preserves the redox ability of W 18 O 49 /ZnO composite photocatalyst. The conversion of aniline reaches 99.1% after 5 h reaction under visible light irradiation at room temperature with an N -formylaniline selectivity of 100%. A possible photocatalytic reaction mechanism is proposed. This study paves a promising way for the design of highly efficient photocatalyst and the sustainable utilization of CO 2 .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Adil Raza,Azhar Ali Haidry,Zhengjun Yao,Talha Amin,Muhammad Ahsan,Razan A. Alshgari,Saikh Mohammad
It is shown that replacing non-noble metals with noble metals in photocatalytic water splitting is pivotal for increased and sustained hydrogen production. However, the challenge persists in designing and developing a cost-effective, highly active catalyst with effective carrier separation and providing sufficient H + reduction sites to enhance photocatalytic H 2 evolution efficiency. Herein, a series of S-scheme Cu 2 ZnSnS 4 /g-C 3 N 4 (CZTS/CN) heterojunction composites were prepared via the hydrothermal method, followed by comprehensive characterizations for in-depth investigation. The TEM image exhibits a clear interface, showing the heterojunction formation between CZTS and CN nanosheets. The results show that incorporating CZTS cocatalyst significantly improves CN photocatalytic hydrogen evolution reaction (HER) and its performance is notably influenced by CZTS to CN mass ratio. Among CZTS/CN heterojunction composites, the 5% CZTS/CN heterojunction composite exhibited a significantly improved HER of 243.64 μmol g −1 h −1 , which is 29.4 and 7.08 folds superior as compared to CN (8.29 μmol g −1 h −1 ) and CZTS (34.42 μmol g −1 h −1 ), respectively. The mechanism study revealed that the excellent superior H 2 evolution performance resulted from the established internal electric field (IEF) in p-n heterojunction, which expedites the efficient separation and migration of photoinduced carriers coupled with the distinctive flower-like configuration of CZTS offering a substantial surface area and enough active reduction sites for photocatalysis process. This work presents a rational design and an inexpensive and efficient heterojunction photocatalysis system suitable for diverse applications.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Xin Liu,Qing Wang,Zhuanxia Zhang,Liangchun Jia,Zhenxing Shen,Tengwen Long,George Zheng Chen,Jun He,Xin Song
The co-mingled plumes of chloroethenes and per- and polyfluoroalkyl substances (PFASs) raise a major challenge for groundwater remediation. This study is the first try to apply sulfidated nano zero-valent iron supported on calcined layered double oxides (S-nZVI@LDO) for simultaneous removal of trichloroethylene (TCE) and perfluorooctanoic acid (PFOA). Our findings revealed that 2 g/L S-nZVI@LDO simultaneously removed 73.3 % TCE and 37.8 % PFOA in pure water, with 49.5 % TCE degraded to less chlorinated products and 23.8 % adsorbed or unquantified transformation of C 3 –C 6 hydrocarbons. Comparative experiments using individual and co-occurring TCE and PFOA revealed that co-existing PFOA and TCE minimally affected their respective removal efficiencies, highlighting S-nZVI@LDO’s suitability for co-contaminant remediation. Furthermore, S-nZVI@LDO achieved optimal TCE and PFOA removal under acidic conditions, surpassing non-composite S-nZVI and LDO. Based on the characterization of S-nZVI@LDO, TCE removal involved reductive dechlorination and sorption via hydrophobic interactions, while PFOA removal was primarily driven by electrostatic interactions and hydrogen bonding. In real groundwater, S-nZVI@LDO achieved 58.2 % TCE and 33.7 % PFOA removal. Additionally, S-nZVI@LDO simultaneously removed nine different PFASs from a 12-PFASs mixture and demonstrated greater effectiveness for long-chain PFASs and their alternatives (e.g., GenX) owing to their hydrophobic nature. These findings highlight the potential of S-nZVI@LDO as an effective material for TCE-PFOA co-contaminated groundwater.
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ChemSusChem
·
2019
·Vol. 12
·期 14
·3390-3400
·
IF 7.804
Nan Jia,Jing Liu,Yunshan Gao,Pei Chen,Xinbing Chen,Zhongwei An,Xifei Li,Yu Chen
Graphical Bifunctional electrocatalyst : A nanocomposite with graphene-encapsulated Co 9 S 8 nanoparticles loaded on N,S-codoped carbon nanotubes is fabricated as a highly efficient and stable bifunctional electrocatalyst for the oxygen reduction and evolution reactions. It can be used as the air electrode in the rechargeable Zn–air battery. An inexpensive and efficient bifunctional electrocatalyst for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is central to the rechargeable zinc–air battery. Herein, a nanohybrid, in which N,S-codoped carbon nanotubes were decorated with Co 9 S 8 nanoparticles encapsulated in porous graphene layers, was fabricated by a one-step heat-treatment process. The N,S dopant species were the major active sites for the ORR, and Co 9 S 8 nanoparticles were mainly responsible for the OER. Compared with commercial 20 wt % Pt/C and Ir/C electrocatalysts, this nanohybrid exhibited a comparable ORR half-wave potential (0.831 V vs. reversible hydrogen electrode) and OER potential (1.591 V at 10 mA cm −2 ), better long-term stability in an alkaline medium, and a narrower potential gap (0.76 V) between ORR and OER. Furthermore, as air electrode of the rechargeable zinc–air battery, it delivered a low charge–discharge voltage gap (0.65 V at 5 mA cm −2 ), high open-circuit potential (1.539 V), good specific capacity (805 mA h g at 5 mA cm −2 ), and excellent cycling stability (48 h), superior to those of commercial Pt/C and Ir/C catalysts, and thus showed promise for applications in renewable energy conversion devices.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xiaohui Song,Rui Huang,Xin Liang,Yang Wang,Qian Hou,Binghui Ge,Qiaobao Zhang,Febri Baskoro,Afriyanti Sumboja,Rong Xiang,Hongfa Xiang,Zhimei Huang
The commercialization of Li-S batteries is constrained by the unstable interface, severe shuttle of polysulfides, and sluggish kinetic conversion reactions. Electrolyte regulation is a straightforward and efficient way to tackle those mentioned issues. Herein, a multifunctional electrolyte additive of 2,5-Dimercapto-1,3,4-thiadiazole (DMTD) is introduced in the ether-based electrolyte, which can be lithiated into Li 2 -DMTD when contacted with the Li or Li 2 S during the discharge process. The generated Li 2 -DMTD can operate as a highly ionic-conducting protective coating on the Li surface, inhibiting the formation of Li dendrites, and increasing interface stability. Then, it is reversibly oligomerized with Li 2 S, forming two organosulfur oligomers during the ensuing electrochemical process. Such a modified reaction routine can reduce the shuttle effect and speed up the reaction kinetics of Li 2 S at the cathode, preventing cathode passivation and boosting active material utilization. As a result, The Li||Li symmetric cells with DMTD exhibit about 5-fold cycle life than the reference cell under 5 mA cm −2 current density. Meanwhile, the initial charge voltage of Li||Li 2 S battery is greatly decreased from 3.7 V to 3.0 V with DMTD, and the assembled Li-S cell shows an improved capacity retention from 45.7 % to 81.2 % after 320 cycles. Therefore, this work successfully tackled the critical issues by designing functional organosulfur electrolyte additives in LSBs, which provides theoretical guidance for the electrolyte design in LSBs.
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Journal of Building Engineering
·
2025
·
IF 7.4
Juanhong Liu,Yayun Xi,Fanghui Han,Lingzhi Guo,Jinmei Hu
This study investigates the influence of aluminum incorporation on the chemical composition, morphology, silicate chain structure, and functional groups of C(-A)-S-H gel through micro- and nanoscale characterization. Based on experimental data, an atomic-scale structural model was constructed to closely reflect realistic Ca/Si and Al/Si ratios as well as Q n distributions, and to explore the effects of aluminum content on the mechanical properties and failure mechanisms of C-A-S-H at the atomic level. Results show that at low Al/Si ratios, Al can be effectively incorporated into the C-S-H gel; however, when Al/Si exceeds 0.10, Al-containing secondary phases start to precipitate. Al atoms bridge defects in silicate chains, extend the length of aluminosilicate chains, and form crosslinking structures along the z direction, with the degree of crosslinking increasing with Al content. Simulation results further indicate that Al incorporation restricts the diffusion pathways of interlayer water molecules, thereby enhancing gel structural integrity. Meanwhile, the formation of a three-dimensional crosslinking network substantially improves mechanical performance, significantly increasing Young's modulus and tensile strength in the y and z directions—especially enhancing interlayer cohesion and ductility along the z direction . Under tensile loading, stress-induced hydrolysis and bond depolymerization accelerate bond cleavage and hydroxyl formation within the C-A-S-H.
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