ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Ziyang Xu,Ying Shen,Liang Chen,Chunbo Wang
Direct CO2 hydrogenation from primary carbon sources such as flue gas offers an attractive route for carbon-neutral fuel synthesis, yet the presence of O2 severely impairs catalyst performance due to preferential H2–O2 reactions and subsequent catalyst deactivation. Herein, we report a surface-engineered Ni/γ-Al2O3 (Ni/A) catalyst modified by Cu doping (Ni–Cu1/A), which exhibits enhanced oxygen resistance and sustained CH4 produce under oxidative conditions. Guided by a descriptor τ, defined as the ratio of O2 to CO2 adsorption energies, Cu was identified as an effective dopant to suppress O2 adsorption while preserving CO2 activation. Under a challenging atmosphere containing 6% O2, the optimized Ni–Cu1/A catalyst achieved a CH4 STY of 76.4 mmol gcat–1 h–1, significantly outperforming the undoped Ni/A catalyst, which drops to 63.1 mmol gcat–1 h–1 under the same conditions. Mechanistic analysis reveals that Cu incorporation weakens O2 adsorption by regulation of electronic structure, thereby mitigating exothermic H2–O2 side reactions and stabilizing Ni0 sites. This work presents a practical and scalable strategy for CO2 methanation in the presence of O2, offering a promising approach for direct catalytic conversion of flue gas by leveraging selective surface adsorption and electronic structure modulation.
研究领域:
催化
·
环境化学
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材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Guiru Sun,Qin Zhao,Tong Wu,Wei Lu,Mei Bao,Liqun Sun,Haiming Xie,Jia Liu
The development of self-standing and binder-free O2 electrodes is significant for enhancing the total specific energy density and suppressing parasitic reactions for Li–O2 batteries, which is still a formidable challenge thus far. Here, a three-dimensional foam-like composite composed of Mo2C nanorods decorated by different amounts of N-doped carbon (Mo2C-NR@xNC (x = 5, 11, and 16 wt %)) was directly employed as the O2 electrode without applications of any binders and current collectors. Mo2C-NR@xNC presents a network microstructure with interconnected macropore and mesoporous channels, which is beneficial to achieving fast Li+ migration and O2 diffusion, facilitating the electrolyte impregnation, and providing enough space for Li2O2 storage. Additionally, the coated N-doped carbon layer can largely improve the electrochemical stability and conductivity of Mo2C. The cell with Mo2C-NR@11NC shows a considerable cyclability of 200 cycles with an overpotential of 0.28 V in the first cycle at a constant current density of 100 mA g–1, a superior reversibility associated with the formation and decomposition of Li2O2 as desired, and a high electrochemical stability. On the basis of the experimental results, the electrochemical mechanism for the cell using Mo2C-NR@11NC is proposed. These results represent a promising process in the development of a self-standing and binder-free foam-based electrode for Li–O2 batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Feilin Zhao,Chizhong Wang,Dongdong Wang,Yimeng Yin,Jie Yu,Jinchi Han,Jie Zeng,Huazhen Chang
A series of Cd-doped NiO catalysts were prepared and tested in the N 2 O catalytic decomposition reaction. In comparison with NiO, it was found that the Cd 0.04 Ni catalyst showed higher N 2 O decomposition activity in the temperature range of 300–450 °C with or without O 2 , and lower activation energy (77.8 kJ mol −1 ). The incorporation of Cd into the NiO lattice was verified by X-ray diffraction (XRD) patterns and Raman spectra. This led to the distortion of the original NiO structure and weakened the Ni-O bond. X-ray photoelectron spectroscopy (XPS) results showed that compared with NiO and CdO, Cd 0.04 Ni possessed higher Ni 2+ and Cd (n+1)+ contents, which might have been induced by the electron transfer behavior between CdO and NiO. A possible mechanism for active site regeneration and O 2 desorption over Cd 0.04 Ni was proposed. The Cd 0.04 Ni catalyst also exhibited good resistance to NO and O 2 .
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2020
·
IF 4.302
Runping Wu,Qing Ye,Kai Wu,Hongxing Dai
To improve the removal capacity of NO + O 2 effectively, the alkaline earth metal-doped order mesoporous carbon (A-C-FDU-15(0.001) (A = Mg, Ca, Sr and Ba)) and Mg-C-FDU-15( x ) ( x = 0.001−0.003) samples were prepared, and their physicochemical and NO + O 2 adsorption properties were determined by means of various techniques. The results show that the sequence in (NO + O 2 ) adsorption performance was as follows: Mg-C-FDU-15(0.001) (93.2 mg/g) > Ca-C-FDU-15(0.001) (82.2 mg/g) > Sr-C-FDU-15(0.001) (76.1 mg/g) > Ba-C-FDU-15(0.001) (72.9 mg/g) > C-FDU-15 (67.1 mg/g). Among all of the A-C-FDU-15(0.001) samples, Mg-C-FDU-15(0.001) possessed the highest (NO + O 2 ) adsorption capacity (106.2 mg/g). The species of alkaline earth metals and basic sites were important factors determining the adsorption of NO + O 2 on the A-C-FDU-15( x ) samples, and (NO + O 2 ) adsorption on the samples was mainly chemical adsorption. Combined with the results of (NO + O 2 )-temperature-programmed desorption ((NO + O 2 )-TPD) and in situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) characterization, we deduced that there were two main pathways of (NO + O 2 ) adsorption: one was first the conversion of NO and O 2 to NO 2 and then part of NO 2 was converted to NO 2 − and NO 3 − ; and the other was the direct oxidation of NO to NO 2 − and NO 3 − .
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Fanyu Meng,Lina Guo,Haocheng Zou,Boming Zhu,Fayang Zhou,Yiqing Zeng,Jiayou Han,Jun Yang,Shule Zhang,Qin Zhong
To achieve high NO oxidation efficiency, excessive O 3 must be used, which would lead to the high cost and escape of ozone. Herein, we adopted low cost and environmental-friendly TiO 2 as the catalyst of low concentration O 3 and H 2 O 2 system for high-efficiency NO x oxidation. The Ti sites on TiO 2 were the deprotonation sites of H 2 O 2 and H 2 O into Ti-OOH and Ti-OH species, respectively. We found that the surface of rutile phase TiO 2 had a low concentration Ti-OOH component but a large amount of Ti-OH after contacting with H 2 O 2 solution, thus lots of ·OH and a few O 2 − radicals formed with introducing O 3 molecules. H 2 O 2 solution induced the formation of a large amount of Ti-OOH and Ti-OH species on the anatase phase TiO 2 surface, thus lots of O 2 − generated in the O 3 /H 2 O 2 system. O 2 − and O H radicals could efficiently oxidize NO, in which O 2 − radicals could oxidize NO to NO 3 − in one step with high selectively. Therefore, anatase TiO 2 had better performance in NO x oxidation than rutile phase TiO 2 . The effect of temperature and SO 2 concentration on NO oxidation was also investigated, the results showed that TiO 2 -A/O 3 /H 2 O 2 system promoted NO oxidation at a low temperature and a low concentration of SO 2 .
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Haiqian Zhao,Jiuyang Jia,Jiaxin Ying,Mingqi He,Zekun Sun,Xing Zhang,Zhonghua Wang,Wei Zhou
Utilizing flue gas as feedstock for CO 2 electro−reduction systems is a promising technology to address problems caused by excessive CO 2 emissions. However, the O 2 contained in the flue gas has a significant adverse effect on the CO 2 reduction. Herein, a facile strategy was proposed to suppress the influence of O 2 by constructing a CO 2 −enriched region. N−doping was demonstrated to be an efficient way to enhance CO 2 adsorption selectivity over O 2 on activated carbon. The N−doped activated carbon achieved 3.7 times increase in CO 2 adsorption selectivity over O 2 than that before modification under simulated flue gas atmosphere (75 %N 2 + 15 %CO 2 + 10 %O 2 ). The distinction in adsorption mechanism between CO 2 and O 2 was revealed by quantum chemistry study. The increased polarity of the carbon materials favored CO 2 adsorption and had less impact on O 2 adsorption. The electrostatic interaction between CO 2 and carbon material was demonstrated to be enhanced after the introduction of pyridinic N and pyrrolic N, which led to an improvement in the CO 2 adsorption capacity. The dispersion interaction, which fully regulated O 2 adsorption, was weakened due to the deviation of the O 2 adsorption position. This study provided a reference for the subsequent development of CO 2 selective adsorption materials.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 167
·期 16
·160557
·
IF 4.316
Guange Wang,Tong Wu,Borui Liu,Shanshan Gong,Qing Huang,Yuefeng Su,Feng Wu,Ryan M. Kelly
Considering that lithium-ion battery (LIB) is still an indispensable and important component of energy storage materials, the sustainable post-processing of spent LIBs in labs or enterprises becomes a tricky problem. Herein, a novel scheme is proposed to dissert the recycling of the spent LIBs. The LIB is recycled into Li(Ni0.9Co0.05Mn0.05)O2 (NCM90) cathode material with high specific capacity by introducing an innovative hydrometallurgy-coprecipitation treatment method. The spent LiCoO2 (LCO) cathode material is firstly leached by sulfuric acid, and the leachate is gradient used as the raw materials to resynthesize high-nickel NCM material by adjusting the leachate dosage to about 50%. Interestingly, when the dosage exceeds 50%, the crystal structure aggravates, and Li+/Ni2+ mixing improves. The specific capacity of regenerated battery is 181.4 mAh g−1 at 0.5 C (1 C = 200 mAh g−1) and the capacity retention achieves 93.2% after 100 cycles. The reasons can be attributed to the cation mixing and crystal strucure and the small amount of Al doping. In conclusion, this combined method recycling of LIBs has huge potential value for environment protection and production.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Wujian Zhang,Weijian Ge,Yiping Jin,Mingming Dang,Panpan Zhang,Wenfeng Han,Ying Li,Zongjian Liu,Haodong Tang
Loaded noble metal redispersion is an important way to solve catalyst sintering. However, how to redisperse at low temperatures or carbon-based noble catalysts is a difficult problem. In this paper, we report this phenomenon occurring on PdCu alloy catalysts, where small-sized PdCu alloys can be realized from sintered large-sized PdCu alloys on carbon supports in a CO/O 2 atmosphere. The mechanism of redispersion is elucidated by XPS, TEM and DFT calculations. The main reason for the redispersion is the formation of the PdCuOx intermediate, which can easily migrate to the nearby catalyst surface and then be reduced to smaller PdCu alloy nanoparticles. This work provides a deeper understanding of the redispersion phenomenon and provides certain applications in industry.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhongwei Li,Guochang Song,Xingyu Yang,Qiang Song
Activated carbon can be used to control NO x emissions in low-temperature flue gas, while improving its performance is challenging. NO adsorption on activated carbon was found significantly promoted with the presence of O 2 . Based on the analysis of NO adsorption characteristics under different atmospheres and corresponding desorption characteristics, NO oxidation, NO 2 migration and further conversion on activated carbon are proposed to cause the significant increase in NO adsorption capacity. Quantum chemical calculations conducted on the adsorption and reaction pathways of NO, O 2 , and NO 2 on different carbonaceous models clarified that the pathway of O 2 -promoted NO adsorption on activated carbon can be divided into two stages. In the first stage, O 2 adsorbs on active carbon atoms near the hydroxyl functional group and undergoes an oxidation reaction with gaseous NO to generate NO 2 . In the second stage, the desorbed NO 2 is re-absorbed on the saturated carbon atoms; the N-down adsorption configuration of NO 2 will not convert, while the O-down adsorption configuration of NO 2 will oxidize the active site to form C-O and release NO; the C-O further reacts with the gaseous NO 2 to form NO 3 - which stably remains. There are two types of active sites involved in the pathway. The active carbon atoms near the hydroxyl functional groups mainly play a catalytic role in the oxidation of NO, while the saturated carbon atoms mainly store nitrogen-containing components. The results can help improve the performance of activated carbon in adsorbing NO in low-temperature flue gas.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Runping Wu,Qing Ye,Kai Wu,Shuiyuan Cheng,Tianfang Kang,Hongxing Dai
The alkali metal (M = Na, K, Rb, and Cs)-modified C-FDU-15 (M-C-FDU-15( x ); x was the M/C-FDU-15 M ratio, and equal to 0.01–0.03) samples were prepared through an in situ process, and characterized by means of the TG, XRD, TEM, EDS, N 2 adsorption–desorption, O 2 -TPD, and CO 2 -TPD techniques. The (NO + O 2 ) adsorption mechanism was investigated using the (NO + O 2 )-TPD and DRIFTS techniques. The results show that the sequence of (NO + O 2 ) adsorption performance was Na-C-FDU-15(0.01) (104.1 mg/g) > K-C-FDU-15(0.01) (92.4 mg/g) > C-FDU-15 (76.2 mg/g) > Rb-C-FDU-15(0.01) (65.1 mg/g) > Cs-C-FDU-15(0.01) (62.3 mg/g). The alkali metal was uniformly distributed in C-FDU-15 and its doping enhanced the amount of the basic sites in the sample. Moreover, the optimal Na/C-FDU-15 M ratio was 0.02. (NO + O 2 ) were chemically adsorbed mainly in the forms of nitrite (NO 2 − ) and nitrate (NO 3 − ) on M-C-FDU-15( x ). A more amount of NO was converted to nitrate than to nitrite. There were three key factors of enhancing the (NO + O 2 ) adsorption capacity of C-FDU-15 due to alkali metal doping: the first factor was the increasing of surface area and pore volume of the sample, the second one was the enhancement in amount of the active sites in the sample, and the third one was the smaller alkali metal ionic radius in the sample.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
·
2019
·
IF 5.714
Zhao Yang,Xu Zhang,Siji Pu,Renxiang Ni,Ying Lin,Yong Liu
A novel heterogeneous Fenton-like system (Mg/Fe-O 2 ) which could directly convert oxygen (O 2 ) to hydrogen peroxide/hydroxyl radicals (H 2 O 2 / • OH) was developed and used to degrade 4-chlorophenol. The Mg/Fe bimetallic particles were prepared by chemical displacement process and characterized by XRD, SEM and TEM. The in situ continuous production of H 2 O 2 / • OH and the effect of the mole ratio of Mg to Fe in the Mg/Fe bimetallic particles and the operating parameters on the degradation 4-chlorophenol in Mg/Fe-O 2 system were investigated in detail. It was found that the Mg/Fe bimetallic particles with the mole ratio of Mg to Fe of 32:1 had the best performance for the 4-chlorophenol degradation and the maximum cumulative concentration of H 2 O 2 , the degradation efficiency of 4-chlorophenol and the removal efficiency of TOC in Mg/Fe-O 2 system were 34.5 mg/L, 100% and 91.8%, respectively, at pH 3, O 2 flow rate 400 mL/min, dosage of Mg/Fe bimetallic particles 2 g/L, 4-chlorophenol initial concentration 50 mg/L and reaction time 60 min. It was revealed by radical scavenging experiments that • OH, particularly the surface-bound • OH, were the predominant reactive oxygen species in Mg/Fe-O 2 system for the degradation of 4-chlorophenol. The main intermediates of 4-chlorophenol degradation were detected by high-resolution liquid chromatography equipped with time-of-flight mass spectrometry (HRLC–ToF-MS) and ion chromatography (IC). Based the results of control experiments and the electrochemical tests, the possible pathway and mechanism of 4-chlorophenol degradation in Mg/Fe-O 2 system were tentatively proposed.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2021
·Vol. 32
·期 2
·2026-2040
·
IF 2.478
Zhang He,Qian Jianhua,Zhang Jie,Xu Jiasheng
TiO 2 @Sn(Sb)O 2 core–shell composites (TiO 2 @SnO 2 , TiO 2 @Sb 2 O 4 and TiO 2 @Sb-SnO 2 ) have been prepared through a chemical co-precipitation method with a calcination process. The mixture hydrolysates of SnCl 4 and SbCl 3 have been deposited on the surface of TiO 2 as the precursor. These hydrolysates have been converted to Sn(Sb)O 2 particles, leading to the formation of the TiO 2 @Sn(Sb)O 2 core–shell structure. Their electrochemical performances and electrocatalytic degradation efficiencies of methylene blue (MB) have been investigated. It is found that TiO 2 @Sb-SnO 2 electrode presents a larger effective electrocatalytic area and more electroactive sites, which provide more contact points between the pollutant and electrode and enhance electrocatalytic oxidation activity. The TiO 2 @Sb-SnO 2 electrode exhibits a higher degradation efficiency (97.6%) than that of TiO 2 @SnO 2 (80.1%) and TiO 2 @Sb 2 O 4 (34.9%). The TiO 2 @Sb-SnO 2 electrode provides a 91.1% degradation efficiency after five cycles test, indicating a high stability during degradation process. These results show that the as-prepared TiO 2 @Sb-SnO 2 electrode can provide a promising application to treat dye wastewater, which relies on its core–shell structure.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）