CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Rui Guo,Yan He,Tao Yu,Peng Cheng,Junhua You,Hongji Lin,Chien-Te Chen,Tingshan Chan,Xuanwen Liu,Zhiwei Hu
Surface modification of electrocatalysts is a convenient strategy for addressing the drawbacks arising from the sluggish kinetics of the oxygen evolution reaction (OER). However, the preparation of electrocatalysts usually involves complex procedures, rendering investigation of the catalytic mechanism difficult. In this study, S-modified FeOOH electrocatalysts were prepared via a facile hydrothermal method at 120 °C. The electrocatalyst exhibited an outstanding OER performance with an overpotential of 254 mV at 50 mA·cm −2 . Morphological, structural, and electrochemical characterizations revealed that Fe ion is the most important active center. The effect of S on the catalytic process was investigated based on the steric hindrance for OH* adsorption, changes in ΔG of the rate-determining step, and coordination mode of the active species. This is the first report on the formation of an (Fe-S)-O* bond that plays a key role in enhancing the electrochemical performance.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiaxin Luo,Yang Qin,Dongbin Zhang,Tong Dou,Meina Tan,Fazhi Zhang,Xuhui Zhao,Yiping Wang,Lirong Zheng,Xiaodong Lei
Due to the modification of anions, an electron redistribution occurs at the metal ions can affect the electronic structure, and induce excellent specific capacity. Herein, we report an effective and low time-consuming method by in-situ wet chemical reduction at room temperature to construct S-modified Cu/Cu 2 O negative electrode material. Moreover, the sulfur can occupy partial O sites in Cu 2 O to play a crucial role in the electronic structure of the material, demonstrated by DFT calculation, XRD, XPS and XAS measurements. The prepared S-Cu/Cu 2 O samples exhibit excellent electrochemical performance with high specific capacity of 669 mAh·g −1 at 1 A·g −1 , even 450 mAh·g −1 at 10 A·g −1 . When the materials are composed as pseudo capacity-type cathode//battery-like anode (MnO 2 //S-Cu/Cu 2 O), and (+) battery-type//battery-type (-) (Ni-Cu hydroxide/Cu(OH) 2 /CF//S-Cu/Cu 2 O) hybrid capacitors, they show the energy density of 47.7 and 147.3 Wh·kg −1 at the power density of 636.2 and 800 kW·kg −1 , respectively. Otherwise, the flexible MnO 2 //S-Cu/Cu 2 O hybrid capacitor is assembled, which also exhibits good performance at different bending conditions. This work can provide a simple method to prepare the electrode materials via in situ anion modification for high-energy density battery-like energy storage systems.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 39
·期 6
·921-927
·
IF 2.726
Li Lingling,Xu Jinhui,Liang Xi,Wu Xueting,Wang Xiao,Song Shuyan,Zhang Hongjie
G old(Au) nanoclusters supported on various supports have been widely used in the fields of energy and catalysis. However, the poor thermal stability of Au nanoclusters on the support interface usually leads to a reduction or even loss of catalytic activity. Herein, we used an in situ reduction method to synthesize Au nanoclusters on ceria(CeO 2 ) carriers. In this method, sulfhydryl groups were used to modify CeO 2 nanospheres first, and then Au clusters with an average diameter of 1.5 nm were grown on the surface of ceria reduced with sodium borohydride. The presence of the Au-S-Ce structure enhances the electron transfer efficiency, making the material exhibit high CO oxidation activity at room temperature. Furthermore, due to the strong binding energy of S and Au, the material exhibits a high stability for long time running process. This strategy provides an idea for designing stable and active supported ultrasmall Au nanoclusters catalytic materials.
研究领域:
催化材料
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能源科学
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2024
·
IF 3.5
Ma Shuwen,Zhu Binji,Gan Ruihui,Wang Yue,Zhou Bangguo,Shi Jingli,Song Yan,Shao Xiaodong,Ma Chang
The development of highly active non-precious metal bifunctional oxygen catalysts is of great significance in improving the efficiency of zinc-air batteries (ZABs). In this work, Co 3 O 4 is modified by a simple sulfur-doping strategy, which achieves a sulfur-doped Co 3 O 4 (S-Co 3 O 4 ) with significantly-enhanced oxygen catalytic activity. The doping of sulfur promotes the exposure of cobalt active sites and brings abundant oxygen vacancies, which provide additional active sites and enhance the conductivity of Co 3 O 4 . Consequently, S-Co 3 O 4 exhibits a low overpotential of 318 mV in the oxygen evolution reaction (OER) and an improved half-wave potential (0.788 V) for oxygen reduction reaction (ORR). In addition, the sulfur doping increases the ORR kinetic current density of pristine Co 3 O 4 by a factor of 49. The assembled ZABs based on S-Co 3 O 4 cathodes show a higher peak power density (98.90 mW cm −2 ) than the commercial Pt/C + RuO 2 -based ZABs. This work reveals that the intrinsic oxygen catalytic activity of Co 3 O 4 can be significantly strengthened by sulfur doping, which can modify its structural characteristics and introduce structural defects. Graphical abstract
研究领域:
材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL SCIENCES
·
2022
·Vol. 134
·期 3
·1-9
·
IF 2.15
Bao Wanting,You Junhua,Zhao Yao,Wang Lu,Yao Ruyue
Electrochemical water splitting has excellent application prospects in clean energy technology. However, due to the large overpotential required for the OER reaction during the water-splitting reaction, the modification of electrocatalysts is a vital strategy to address the slow kinetics of the OER reaction. In this paper, a simple and rapid two-step hydrothermal sulfidation method was used to prepare S-modified Ni(OH) 2 nanosheets electrocatalysts at 120 °C. At the same time, the well-designed nanostructured catalyst on the nickel foam substrate exposes a large number of active sites, and the simultaneously generated oxygen vacancies are beneficial to the penetration of the electrolyte and release of O 2 , thus significantly improving the OER performance. In 1.0 M KOH electrolyte, Ni 9 S 8 /Ni(OH) 2 /NF exhibits excellent catalytic activity for OER. The catalyst requires only 430 mV overpotential at a current density of 100 mA cm -2 . In addition, Ni 9 S 8 /Ni(OH) 2 /NF also has excellent long-term stability. Graphical abstract This work reports the formation of Ni 9 S 8 /Ni(OH) 2 /NF heterojunctions by sulfiding Ni(OH) 2 on porous nickel foam. Surprisingly, these Ni 9 S 8 /Ni(OH) 2 /NF heterojunctions exhibit excellent oxygen evolution reaction performance and long-term stability. This is superior to most reported electrocatalysts for oxygen evolution reactions.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 29
·23819-23826
·
IF 4.6
Yanhong Ding,Zhichao Gao,Rongpeng Lin,Yong Cao,Haoyang Liu,Yulin Zhou,Haifeng Xu,Jiayi Liu,Fangqi Ren,Yirong Zhu
Lithium–oxygen (Li–O2) batteries are considered an important candidate for the next generation of energy storage systems due to their ultra-high theoretical energy density (11 586 mA h g−1), but their slow kinetic reactions, high overpotential and cyclic instability seriously limit their practical applications. In this study, sulfur modified Mo2C (S@Mo2C) cathode materials were prepared by hydrothermal synthesis by sulfur (S) doping to optimize the electronic structure and catalytic activity of Mo2C (Mo2C). Experiments show that S@Mo2C exhibits significantly improved electrochemical performance compared to commercial Mo2C: its specific capacity is up to 3955 mA h g−1 (commercial material only 508 mA h g−1), the charge and discharge overpotential is reduced to 0.26 V (53.6%), and the capacity retention rate remains 77.8% after 250 cycles. X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) analysis showed that the introduction of sulfur induced the formation of a heterostructure of MoS2/MoS3 in the Mo2C lattice, which enhanced the conductivity and oxygen reduction/precipitation (ORR/OER) activity of the material. In addition, sulfur doping promotes the formation of highly conductive amorphous Li2O2 and effectively inhibits the accumulation of insulating ring Li2O2, thus significantly improving the cycle stability and energy efficiency of the battery. This study provides a new structural regulation strategy for the design of high efficiency lithium oxygen battery catalysts.
研究领域:
能源存储
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材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 41
·14439-14447
·
IF 6.4
Qingling Zhao,Xiaotong Wang,Qinghong Song,Zehao Zang,Chunyan Fan,Lanlan Li,Xiaofei Yu,Zunming Lu,Xinghua Zhang
Multicolor emissive carbon dots (CDs) hold great potential for a wide range of applications in various fields. However, the luminescence enhancement mechanism is still controversial due to combined effects of the carbon core and surface states. Herein, we elucidate the surface state mechanism for the tunable and enhanced photoluminescence of CDs via only surface nitrogen and sulfur modification (N,S-CDs) through an electrochemical synthesis method. It is demonstrated that surface nitrogen functionalization with increasing content of NH2 groups leads to multicolor emission from blue to red. Moreover, surface sulfur functionalization with the introduction of C–S bonds can further improve the luminescence intensity by facilitating the transition of S-related excitation electrons and radiative recombination. In addition, the high luminance of N,S-GCDs enables their application in flexible fluorescence films, latent fingerprint detection and information encryption.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Water Research & Technology
·
2025
·
IF 3.1
Kunlun Yang,Yimei Wang,Dengyang Wang,Zengshuai Zhang,Peng Gu,Xueli Ren,Hengfeng Miao
Combined with the separation and dehydration treatment of digestate from anaerobic digestion and acidification of food waste, sulfur-modified digestate biochar was facilely prepared for efficient Cr(VI) removal to realize anaerobic digestate recycling and waste control by waste. Characterization indicated the increased surface area and mesopores and the decreased aggregation degree for biochar under optimized S doping and pyrolysis temperature (900-2S@DBC), resulting in more functional groups with high reducibility (e.g., phenolic -OH, C-S-C, S species with low valency) and improved electron transfer ability. The forms transformation analysis confirmed the reduction of sulfate source via carbon under high pyrolysis temperature. Under the conditions of an initial Cr(VI) concentration of 10 mg/L, a pH of 3, and a dosage of 0.5 g/L, the removal efficiency of Cr(VI) by 900-2S@DBC approaches 100%. 900-2S@DBC showed apparent higher Cr(VI) removal performance than other biochar. Its quasi-second-order kinetic constant was tens of times than pristine biochar. Quenching and control experiments confirmed the S species with low valency played a more important role in Cr(VI) reduction than traditional carbon and oxygen based reductive groups on carbon structure. Direct surface electron reduction made more contribution than indirect solution •O2- reduction pathway, further confirming the synergistic effect between Cr(VI) sorption and reduction. Complexation, precipitation, and ion exchange processes participated in the final immobilization of Cr by 900-2S@DBC. Additionally, 900-2S@DBC exhibited excellent Cr(VI) removal capacity in real electroplating wastewater. This study offered a feasible approach for resource utilization of anaerobic digestate and deep insights for Cr(VI) removal mechanism via sulfur-modified biochar.
研究领域:
环境科学
·
废弃物资源化
·
污染控制
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yaqian Dong,Zhi Fang,Deliu Ou,Qing Shi,Yu Ma,Weiyou Yang,Bin Tang,Qiao Liu
Constructing inexpensive, efficient, and stable pH-universal oxygen reduction electrocatalysts with controlled distribution of active species is of great importance for the exploration of green energy conversion devices. Herein, we demonstrated the rational preparation of S-modified Fe–N–C nanosheet catalysts with hierarchical porous architecture, large specific surface area (up to 1471 m 2 g −1 ) and controlled S doping (up to 12.3 at.%) by the co-pyrolysis of cysteine, FeCl 3 with Zn-mediated MgO template. Merited from rich and accessible active sites, the catalysts display outstanding oxygen reduction reaction (ORR) activity in terms of very small E j3 (potential@3 mA cm −2 , 0.87 V in 0.1 M KOH, 0.66 V in 0.1 M PBS (pH7.4) and 0.64 V in 0.5 M H 2 SO 4 ) and overwhelming diffusion-limited current density (9.8, 6.1, 10.3 mA cm −2 in alkaline, neutral, acidic media, respectively), along with extremely respectable stability (∼90% activity retention for 53200, 26728, 43200 s in alkaline, neutral, acidic media, respectively), which underscore comparable or even better overall performance than commercial Pt/C and advanced pH-universal ORR catalysts ever reported. The as-assembled primary alkaline zinc–air battery delivers considerately large peak power density of 205 mW cm −2 and energy density up to 990.6 Wh kg Zn −1 at 10 mA cm −2 (115 mW cm −2 and 676.7 Wh kg Zn −1 for Pt/C-based battery), implying its highly promising application in practical energy conversion devices.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 5
·3541-3550
·
IF 3.201
Ruyi Fang,Chengwei Lu,Wenkui Zhang,Zhen Xiao,Hongfeng Chen,Chu Liang,Hui Huang,Yongping Gan,Jun Zhang,Yang Xia
A novel synthetic strategy has been successfully developed, which utilizes supercritical CO2 (SC-CO2) to fabricate sulfur-modified zeolites (zeolites@S) for Hg2+ removal from water. Owing to the low viscosity, high diffusivity and excellent dissolving capacity of SC-CO2 as well as the nontoxicity, noninflammability and being a low-cost solvent it exhibits the strong ability to expand the crystal structure of zeolite and the high-efficiency transfer of sulfur in zeolite matrices. Benefiting from this unique microstructure, zeolites@S adsorbents provide abundant pores and voids for absorbing Hg2+, and synchronously offer extra active sites for chemically trapping Hg2+ with sulfur. The pseudo-first-order kinetic/pseudo-second-order kinetic models and Langmuir/Freundlich isotherm models have been employed to study the adsorption behaviors and adsorption kinetic parameters. The results demonstrated that zeolites@S-15 (sulfur content = 15 wt%) exhibited the highest adsorption capacity and the best kinetic parameters for Hg2+ relative to other samples. This work will not only provide important reference for the rational design of zeolite based adsorbents for Hg2+ removal from aqueous solution, but also pave a new way to boost the commercialization of low-cost and high-efficiency functionalized adsorbents for purifying wastewater.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Yong Yuan,Haomiao Xu,Wei Liu,Lihong Chen,Zongwen Quan,Ping Liu,Zan Qu,Naiqiang Yan
Porous structure and effective active site are beneficial for gaseous elemental mercury (Hg 0 ) capture. Two kinds of hierarchical porous layered double hydroxides (LDHs) were synthesized through an in-situ growth method. Sulfur was used for the modification of these LDHs to enhance Hg 0 removal performance. Two as-prepared NiAl-S 4 @SiO 2 microspheres displayed three-dimensional morphologies, accordingly exhibited as core-shell and urchin-like morphologies. XRD , BET, FTIR, TEM and SEM were employed to investigate the structure effect on Hg 0 uptake. The results indicated that after S-modification, the Hg 0 removal efficiencies as well as SO 2 resistance were enhanced. The Hg 0 removal performances follow the order of: NiAl-S 4 @SiO 2 -urchin > NiAl-S 4 @SiO 2 -core at 100 °C. The mechanism for Hg 0 removal was discussed based on the results of TPD , EDX and XPS . The porous structure of NiAl-S 4 @SiO 2 composite was beneficial for gas transformation and intercalated [S 4 ] 2− ions were favorable for mercury uptake. The polysulfide combined with adsorbed mercury and formed HgS. Such materials exhibit promising potential for mercury uptake from S Hg mixed flue gas.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 1
·1-11
·
IF 2.9
Zhang Kai,Chen Yang,Fang Zhanqiang
The problems of biochar such as low adsorption capacity and slow adsorption rate limit its application in removing cadmium from water. However, the modification for enhancing the efficiency and expanding the application of biochar is a good way. In this paper, sulfur-modified biochar (SBC) derived from bagasse was prepared by impregnation pyrolysis at 500 °C. Sulfur was successfully loaded on the surface of biochar by SEM–EDS analysis and the specific surface area of SBC could be significantly increased by BET analysis. Batch experiments showed that the cadmium removal efficiency by SBC could reach more than 90% within 10 min, and the maximum adsorption capacity of cadmium was 268.2 mg g −1 , which was 22.35 times as high as that of unmodified biochar. Ion exchange with Na + , surface precipitation (CdCO 3 and CdS), complexation with C-SH, S–O, and COOH, and electrostatic interaction were the main mechanisms by XRD, FT-IR, and XPS analysis.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）