JOURNAL OF MATERIALS SCIENCE
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2021
·Vol. 56
·期 19
·11426-11435
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IF 4.22
Yan Dong,Peng Zhen,Wang Wei,Zeng Peng,Huang Yiyin
Abstract Carbon-based metal-free catalysts exhibit great applications in electrochemical CO 2 reduction (ECR), while most studies merely focus on large-sized carbons with limited ratio of surface atoms for engineering to create surface active centers. Here, we report a joint treatment of C60 by heating and plasma to induce a dramatic performance promotion during ECR. The electrochemical measurements indicate the Faraday efficiency for ECR toward CO production kept at high level over 80% in a wide potential region from − 0.4 to − 0.7 V versus RHE, with the highest value reaching 96.8%. The physical characterization reveals that fragmentation of C60 occurs together with N/O doping, both of which could induce change in electron structure, causing the formation of *COOH intermediate and ultimately leading to the optimized activity and selectivity for CO production. This treatment route was further revealed to be applicative for other carbon materials, e.g., single-walled carbon nanotube, to promote its ECR activity and selectivity. Graphical Abstract
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
Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Shangguan Wenchao,Liu Qing,Wang Ying,Sun Ning,Liu Yu,Zhao Rui,Li Yingxuan,Wang Chuanyi,Zhao Jincai
Achieving CO 2 reduction with H 2 O on metal photocatalysts and understanding the corresponding mechanisms at the molecular level are challenging. Herein, we report that quantum-sized Au nanoparticles can photocatalytically reduce CO 2 to CO with the help of H 2 O by electron-hole pairs mainly originating from interband transitions. Notably, the Au photocatalyst shows a CO production rate of 4.73 mmol g −1 h −1 (~100% selectivity), ~2.5 times the rate during CO 2 reduction with H 2 under the same experimental conditions, under low-intensity irradiation at 420 nm. Theoretical and experimental studies reveal that the increased activity is induced by surface Au–O species formed from H 2 O decomposition, which synchronously optimizes the rate-determining steps in the CO 2 reduction and H 2 O oxidation reactions, lowers the energy barriers for the *CO desorption and *OOH formation, and facilitates CO and O 2 production. Our findings provide an in-depth mechanistic understanding for designing active metal photocatalysts for efficient CO 2 reduction with H 2 O.
研究领域:
化学
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材料科学
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环境科学
·
催化
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DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yulan Xu,Minxian Wu,Xianxian Zhang,Wenchang Wang,Naotoshi Mitsuzaki,Zhidong Chen
Electrodeposition is a simple and rapid method for the preparation of thin-film materials, allowing catalytic materials to be directly deposited onto substrates, thereby eliminating the need for binders. Compared with bulk materials, two-dimensional thin films possess a higher specific surface area. The incorporation of Ga in Sn-based alloy materials can effectively expose active sites, thereby enhancing the catalytic performance for CO 2 electroreduction. Doping with rare-earth elements such as cerium can induce the formation of oxygen vacancies and defect sites, or modulate the electronic structure of the catalyst surface. These modifications enable independent regulation of the adsorption energy of various intermediates, effectively lowering reaction energy barriers and improving catalytic efficiency. In this work, Ga-Sn-Ce electrodes were synthesized via electrodeposition in a deep eutectic solvent composed of choline chloride and urea, and subsequently applied to CO 2 reduction. The GaSnCe0.6 electrode exhibited excellent selectivity toward formic acid at −0.99 V vs. the reversible hydrogen electrode, achieving a Faradaic efficiency of 92 %. Compared with previously reported Ga-Sn alloys, the introduction of Ce resulted in a positive shift of 250–270 mV in the optimal reduction potential for formic acid production from CO 2 .
研究领域:
催化化学
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材料科学
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电化学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Mingmin Jia,Xiong-Fei Zhang,Yicheng Zhou,Hengyang Mao,Yijiang Zhao,Jianfeng Yao
In this work, Amine-functionalized CNF/UiO-66 (CNF–NH 2 /UiO-66) composite membranes were fabricated by incorporating UiO-66 nanoparticles in the CNF–NH 2 matrix. The CO 2 -facilitated transfer channels can be constructed in the CNF–NH 2 /UiO-66 composite membrane. As a natural polymer material, CNF–NH 2 would absorb water and form a gel-like structure under humidification. The adsorbed water can convert CO 2 into bicarbonate ions (HCO 3 − ) through the catalysis of amino groups on CNF–NH 2 . Moreover, in CNF–NH 2 /UiO-66 composite membranes, HCO 3 − could quickly migrate to the permeate side promoted by the porous UiO-66, facilitating CO 2 transport. The optimum membrane gave a CO 2 permeability of 257.0 Barrer with a CO 2 /CH 4 ideal selectivity of 71.3.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Nan Kong,Huiling Du,Zhuo Li,Tong Lu,Siyu Xia,Ziwei Tang,Shijie Song
Metal-organic frameworks (MOFs), featuring semiconductor-like behavior, are promising for the photocatalytic reduction of CO 2 . While their practical application is hindered by the disadvantages of low charge migration efficiency and fast electron-hole pair complexation. In this paper, a simple solvothermal method was used to load NH 2 -UiO-66 onto the surface of MIL-101(Cr) to form a nano type II heterojunction double MOFs composite of NH 2 -UiO-66 @MIL-101. The results show that the heterostructure of NH 2 -UiO-66 @MIL-101 promotes the separation of photogenerated electron-hole pairs and accelerates the interfacial photogenerated electron transfer under light, and the NH 2 -UiO-66 @MIL-101 type II heterojunction exhibits higher activity for photocatalytic reduction of CO 2 compared with pure MIL-101(Cr) and NH 2 -UiO-66. In addition, the possible photocatalytic mechanism was further elucidated to demonstrate the increased photocatalytic activity of NH 2 -UiO-66 @MIL-101. This study provides effective insights for designing efficient MOFs photocatalysts for CO 2 reduction to enhance the photocatalytic activity for environmental protection and governance.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xin Li,Jingru Guan,Haopeng Jiang,Xianghai Song,Pengwei Huo,Huiqin Wang
Construction of multi-interface contact step-scheme (S-scheme) photocatalyst is a promising pathway to achieve high-electron transfer efficiency for photocatalytic CO 2 reduction. In this paper, g-C 3 N 4 nanosheets were selected as the main photocatalyst, rod-like CeO 2 (R-CeO 2 ) with unique Ce 4+ →Ce 3+ conversion property and rGO were loaded on the g-C 3 N 4 surface to construct 2D-1D-2D sandwich photocatalyst. The yields of CO and CH 4 were about 63.18 and 32.67 μmol/g after 4 h when the rGO/R-CeO 2 /g-C 3 N 4 was used as catalyst, which were about 4 and 6 times higher than that of pure CN, respectively. Cyclic experiments proved that the composite had excellent photocatalytic and material stability. Photoelectrochemical tests showed that the construction of S-scheme electron transfer model and the introduction of rGO can great enhance the electron transmission and separation of photogenerated electron-hole pairs. CO 2 adsorption test identified that the loading of R-CeO 2 and rGO obviously enhanced the CO 2 adsorption ability of pure g-C 3 N 4 . Density functional theory (DFT) calculations used to analyze the electron transfer path and the formation of the build-in electric field at the semiconductor interface. In-situ FTIR and 13 CO 2 element-tracer detection carried out to research the process of CO 2 photoreduction. A possible multi-interface contact S-scheme electron transfer mechanism for enhanced CO 2 photoreduction activity has been discussed.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2016
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IF 2.567
Teng Lu,Zhaomin Li,Weiyu Fan,Xinglu Zhang,Qichao Lv
The deposition of asphaltenes in porous media is one of the most difficult problems during CO2 flooding. In this paper, the adsorption of asphaltenes onto Al2O3 nanoparticles was studied through two methods: (i) by adding a certain mass of nanoparticles in a fixed volume of solution with different initial concentrations of asphaltenes and (ii) by exposing a certain amount of asphaltenes in a fixed volume of solution to different nanoparticles additions. Then, the impact of Al2O3 nanoparticles on the asphaltene precipitation was investigated using the IFT behavior of the oil–CO2 system. Coreflood tests were conducted to study the potential of nanoparticles for inhibition of asphaltenes damage during CO2 flooding, and the effect of injection parameters of nanofluid. It is found that the solid–liquid equilibrium (SLE) can well describe the isotherms of asphaltene adsorption. The trend of the IFT–pressure curve is affected by asphaltene accumulation at the oil–CO2 interface. The slopes in the high pressure region can be used to examine the intensity of asphaltene precipitation. As the addition of nanoparticles increases, the IFT slope in the high pressure range decreases. This is because the asphaltenes are absorbed at the surface of nanoparticles. As a result, the nanoparticles prevent asphaltene precipitation from accumulating at the CO2–oil interface, hence causing asphaltene to remain within the bulk of oil. The higher the mass fraction of Al2O3 nanoparticles is, the lower the intensity of the asphaltene precipitation would be. The coreflood results show that the injection of Al2O3 nanofluid can lessen the oil permeability reduction because the nanoparticles can inhibit the deposition of asphaltenes onto the sand surfaces in the porous media. The 0.5 wt % nanoparticles and the 0.1 nanofluid/CO2 slug volume ratio are considered as the optimum for inhibiting asphaltenes damage during CO2 flooding. Continuous CO2 and nanofluid injection could be more effective compared with the cyclic injection pattern.
研究领域:
石油工程
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材料科学
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DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2023
·Vol. 25
·期 33
·21944-21956
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IF 3.3
Zhen Wang,Chenteng Sun,Qian Xu,Xingli Zou,Hongwei Cheng,Xionggang Lu
Alkali and alkali earth oxides show good CO2 capture performance for carbonation, while their regeneration occurs at high temperatures, leading to a high energy penalty. When alkali oxides and alkali earth oxides combine with SiO2 to form oxysalts, the regeneration temperatures can be reduced, and the CO2 adsorption capacity is maintained. In this study, the reaction between CO2 and Li2CaSiO4, composed of stoichiometric CaO, Li2O, and SiO2, was evaluated thermodynamically by DFT. The synthesized Li2CaSiO4 with and without alkali carbonates was used as CO2 sorbents, and their CO2 adsorption performances were examined using thermal analyses. The phase and morphology of Li2CaSiO4 before and after CO2 adsorption were characterized by XRD and SEM. According to the thermodynamic evaluation and the XRD results, Li2CaSiO4 could adsorb CO2 and form CaCO3 and Li2SiO3. The thermal analyses showed that the regeneration of Li2CaSiO4 started from 575 °C, at which it was difficult to realize the CO2 diffusion through the solid CaCO3 product layer. The mixed alkali carbonates can improve the kinetics and facilitate the CO2 adsorption of Li2CaSiO4. Alkali carbonates were effective in reducing the activation energy of the reaction and CO2 diffusion at low temperatures and improving the cyclic stability because of the dispersing carbonation products.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Materials Science & Engineering C-Materials for Biological Applications
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2021
·
IF 7.328
Xiangping Wen,Guangming Wen,Wenyan Li,Zhonghua Zhao,Xine Duan,Wenjun Yan,John F. Trant,Yingqi Li
Fluorescent carbon dots (CDs) were hydrothermally synthesized from a mixture of frozen tofu, ethylenediamine and phosphoric acid in an efficient 64% yield. The resulting CDs exhibit good water solubility, low cytotoxicity, high stability, and excellent biocompatibility. The CDs selectively and sensitively detect Co 2+ through fluorescent quenching with a detection limit of 58 nM. Fluorescence can be restored through the introduction of EDTA, and this phenomenon can be used to quantify EDTA in solution with a detection limit of 98 nM. As both analytes are detected by the same CD platform, this is an “off-on” fluorescence sensor for Co 2+ and EDTA. The technique's robustness for real-world samples was illustrated by quantifying cobalt in tap water and EDTA in contact lens solution. The CDs were also evaluated for in vivo imaging as they show low cytotoxicity and excellent cellular uptake. In a zebrafish model, the CDs are rapidly adsorbed from the intestine into the liver, and are essentially cleared from the body in 24 h with no appreciable bioaccumulation. Their simple and efficient synthesis, combined with excellent physical and chemical performance, renders these CDs attractive candidates for theranostic applications in targeted “smart” drug delivery and bioimaging.
研究领域:
分析化学
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生物医学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Processes
·
2023
·Vol. 11
·期 4
·1075
·
IF 3.5
Zhaochen Huang,Guoqiang Huang
Usually, the ion implantation gases used in semiconductor production are required to be extremely high in purity. Due to the presence of trace CO2in electronic special gas BF3, the quality of the material is significantly affected, which makes it crucial to impose control on CO2content. Unlike a series of blank adsorbents reported in other studies, the zinc-loaded adsorbents prepared in this study are intended for the adsorption of CO2from CO2/BF3. Firstly, the materials were characterized by XRD, BET, SEM-EDS and TG-DSC analysis, etc., and the breakthrough curves of the adsorbents as obtained under different preparation conditions were investigated at 20 °C and 200 kPa. The results show that the adsorption performance reached the optimal level when the activation temperature was 450 °C and a 13X molecular sieve was impregnated by 0.15 mol/L Zn(NO3)2. Moreover, compared with the Zn-13X, the breakthrough time was reduced to 69% and 44% in two adsorption cycles, respectively. Finally, FTIR was used to reveal the adsorption mechanism of the carbonates produced by CO2adsorption. It was found that the adsorption performance was affected by the irreversible reduction in the number of active sites due to the continuous formation of polydentate carbonate during adsorption and regeneration.Keywords:CO2adsorption;13X molecular sieve;carbonate species
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
APPLIED ENERGY
·
2022
·
IF 11.446
Boshu Jiang,Bachirou Guene Lougou,Hao Zhang,Boxi Geng,Lianxuan Wu,Yong Shuai
The solar-driven thermochemical CO 2 -to-CO conversion is an effective way to achieve the mission of carbon peaking and carbon neutrality. However, synthesizing porous reacting materials with excellent thermal stability, hardness and long-term cyclic stability, oxygen exchange capacity, and higher CO 2 -to-CO conversion are the most important challenges associated with the thermochemical CO 2 -splitting approach and technological upscaling to large-scale applications. This study presented the development of NiFe 2 O 4 oxygen carriers, the synthesis method of SiC and Si 3 N 4 supports, and solar-to-fuel processing of the newly prepared materials through CO 2 -splitting under a highly concentrated solar radiative heat flux. The newly synthesized NiFe 2 O 4 @SiC porous redox material resulted in higher solar energy absorption and CO 2 conversion capability with an instantaneous CO production of 410 μmol/g and direct CO 2 -to-CO conversion rate of 18.1 % at 1073–1273 K reaction temperature. The media composite of NiFe 2 O 4 @SiC exhibited high-temperature thermal changes, good thermochemical reaction stability, and a higher CO production rate through six redox cycles compared to NiFe 2 O 4 @Si 3 N 4 porous reacting material. The high oxidation potential and remarkably solar radiative heat flux absorption and thermochemical CO 2 -splitting capacities of the newly developed materials were demonstrated through experimental analysis. The synergistic effect of the oxygen carriers (NiFe 2 O 4 ) and substrate materials including SiC and Si 3 N 4 skeletons for CO 2 -splitting is highlighted. This study provided comprehensive and novel experimental insights that can be used as guidance for theoretical research and application in CO 2 conversion into high-value-added energy products.
研究领域:
材料科学
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可再生能源
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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
·
2016
·Vol. 5
·期 4
·1509-1515
·
IF 8.262
Shaolei Wang,Kunpeng Song,Chengxin Zhang,Yu Shu,Tao Li,Bien Tan
A novel metalporphyrin-based microporous organic polymer (HUST-1-Co), which possesses a high surface area of 1360 m2 g−1 and a high CO2 uptake of 21.39 wt% (1 bar and 273 K) for CO2 capture and storage (CCS) and the efficient chemical conversion of CO2 under ambient conditions, is reported. This polymer incorporated both ultra-micropores and catalytic sites, and was synthesized by a novel solvent knitting hypercrosslinked polymers method, using 5,10,15,20-tetraphenylporphyrin (TPP) as the building block. The N2 sorption isotherms of the polymers show that HUST-1-Co possesses abundant ultra-micropores (centered at 0.68 nm), and a continuous mesoporous and macroporous structure, which not only enhances the interaction between the pore walls and CO2, but is also favourable for the catalysis process. The synergy of the ultra-micropores, abundant nitrogen atoms and Co2+ ions makes HUST-1-Co one of the highest CO2 uptake MOP materials reported so far and further endows it with efficient catalytic performance. HUST-1-Co is one of the most efficient catalysts for the coupling of CO2 with substituted epoxides with various functional groups at room temperature and atmospheric pressure, with an excellent recycling performance (more than 15 times). Moreover, the role of the mesoporous and macroporous structure of HUST-1-Co gives it a unique catalytic performance for different molecular sizes of epoxide substrates with excellent yields (>93%).
研究领域:
材料科学
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环境科学
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化学工程
✓ 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）