CHINESE JOURNAL OF CATALYSIS
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2022
·
IF 12.92
Yue Huang,Kai Dai,Jinfeng Zhang,Graham Dawson
Non-stoichiometric W 18 O 49 (WO) prepared by solvothermal method has excellent NIR absorption due to the localized surface plasmon resonance effect caused by oxygen vacancies. This has great potential in the field of using sunlight to convert carbon dioxide into organic fuels. In addition, through the amination of CdSe, the one-dimensional/two-dimensional step-scheme (S-scheme) WO/CdSe-diethylenetriamine (WO/CdSe-D) photocatalyst with electron transmission channels driven by visible light to NIR light is constructed by microwave solvothermal method. The LSPR of WO and the synergistic effect of coupling semiconductors to construct S-scheme heterojunctions can improve light utilization and achieve efficient charge carrier transfer efficiency. The optimized photocatalyst of 35%WO/CdSe-D has the best CO 2 reduction performance compared to WO and CdSe-D, and the yield is 25.37 µmol h –1 g –1 . X-ray photoelectron spectroscopy was used to verify the charge transfer path of the S-scheme WO/CdSe-D heterojunction. This work provides a possibility for the application of non-stoichiometric oxides rich in oxygen vacancies in the field of photocatalytic CO 2 reduction.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
DOI
高影响因子
Science Advances
·
2023
·Vol. 9
·期 24
·
IF 13.6
Mingrui Wang,Peng Wang,Guanghui Zhang,Zening Cheng,Mengmeng Zhang,Yulong Liu,Rongtan Li,Jie Zhu,Jianyang Wang,Kai Bian,Yi Liu,Fanshu Ding,Thomas P. Senftle,Xiaowa Nie,Qiang Fu,Chunshan Song,Xinwen Guo
The decomposition of cobalt carbide (Co 2 C) to metallic cobalt in CO 2 hydrogenation results in a notable drop in the selectivity of valued C 2+ products, and the stabilization of Co 2 C remains a grand challenge. Here, we report an in situ synthesized K-Co 2 C catalyst, and the selectivity of C 2+ hydrocarbons in CO 2 hydrogenation achieves 67.3% at 300°C, 3.0 MPa. Experimental and theoretical results elucidate that CoO transforms to Co 2 C in the reaction, while the stabilization of Co 2 C is dependent on the reaction atmosphere and the K promoter. During the carburization, the K promoter and H 2 O jointly assist in the formation of surface C * species via the carboxylate intermediate, while the adsorption of C * on CoO is enhanced by the K promoter. The lifetime of the K-Co 2 C is further prolonged from 35 hours to over 200 hours by co-feeding H 2 O. This work provides a fundamental understanding toward the role of H 2 O in Co 2 C chemistry, as well as the potential of extending its application in other reactions.
研究领域:
催化化学
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化学工程
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材料科学
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可持续能源
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多相催化
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
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2019
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IF 8.456
Guanying Dong,Jingjing Zhang,Zheng Wang,Jing Wang,Peixia Zhao,Xingzhong Cao,Yatao Zhang
Polydopamine-modified additives have been thus far widely used in the mixed matrix membranes (MMMs) for gas separation. However, very few reports focus on the polydopamine alone and investigate its contribution to the gas separation performance. Herein, the polydopamine-derived submicrospheres (PDASS) were paired with polymers of intrinsic microporosity (PIM-1) to fabricate high-performance gas separation membranes, through which the effects of PDASS on gas permeability and CO2/N2 separation performance were systematically investigated. The addition of PDASS provides a 1.6-fold enhancement in CO2/N2 selectivity together with acceptable gas permeability as compared to the original polymeric membrane. Such enhanced separation behavior is supposed to stem from the densified membrane microstructure induced by the strong intermolecular interactions between PIM-1 and PDASS (i.e., charge transfer, π–π stacking, and hydrogen bonding). Importantly, the physical aging behavior, as judged by gas permeability, is retarded for PIM/PDASS membranes after 4 months of testing.
研究领域:
材料科学
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化学工程
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膜技术
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气体分离
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2018
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IF 4.439
Pan Li,Chunchao Hou,Xuehua Zhang,Yong Chen,Tao He
The hybrid coupling between inorganic semiconductor and molecular catalyst can provide a promising approach for the construction of highly efficient and selective photocatalytic CO 2 reduction systems. This hybrid system can take full advantage of the strong light harvesting capability of semiconductor and high selectivity of molecular catalyst. The interaction linker bridging the semiconductor and molecular catalyst plays an important role in supplying efficient electron transfer channels. In this study, both CdS with and without ethylenediamine functionalization (i.e., CdS-EF and CdS) have been successfully synthesized and further respectively coupled with tetra(4-carboxyphenyl)porphyrin iron(III) chloride (FeTCPP) for CO 2 photoreduction. It is found that CdS-EF exhibits inferior photocatalytic activity to CdS, while CdS-EF/FeTCPP hybrid photocatalyst shows much higher activity than CdS/FeTCPP. This is because hydrogen bonding exists between the amino groups in CdS-EF and carboxyl groups in FeTCPP, which can act as electron transfer channels from CdS to FeTCPP in the obtained hybrid system.
研究领域:
材料科学
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光催化
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环境化学
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无机化学
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分子催化
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yanwei Sun,Chunshan Song,Xinwen Guo,Yi Liu
Preferred orientation has proven to exert a significant impact on the gas separation performance of metal–organic framework membranes. Nevertheless, realizing three-dimensional orientation control remains a challenging issue. In this study, well-intergrown NH2-UiO-66 membranes with both (111) out-of-plane and regional in-plane orientations were prepared by combining oriented deposition of seeds and solvothermal epitaxial growth. Dynamic air–liquid interface-assisted self-assembly method was employed to organize uniform octahedral-shaped NH2-UiO-66 seeds into closely packed monolayers with (111) out-of-plane and regional in-plane orientations, whereas the use of ZrS2 as the zirconium precursor during the solvothermal epitaxial growth was found indispensible for sealing the intercrystalline gaps while preserving the preferred orientation inherited from seed layers. In addition, compared with solvothermal heating, employing microwave heating led to poor intergrowth between neighboring NH2-UiO-66 crystals because of a lower dielectric loss factor of the reaction medium. Gas permeation results indicated that the prepared NH2-UiO-66 membranes exhibited H2/CO2 selectivity up to 5.5 times higher than their counterparts with random and/or mere out-of-plane orientations as well as H2 permeability 14.5 times higher than NH2-MIL-125(Ti) membranes with mere out-of-plane orientation under similar operating conditions.
研究领域:
材料科学
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化学工程
·
膜技术
✓ 已验证
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Shuai Hu,Xiaoxuan Zhu,Yan Zhu,Chenliang Zhou,Gewen Yu,Yanming Wang,Cong Wang,Zhenfeng Wang,Jian Ding,Yuqing Wang,Xiaohui Guo
To enhance the activity and selectivity of Cu-based catalysts in the CO 2 hydrogenation reaction, this study systematically investigated the regulation effect of Nd-doping on the structure and surface properties of different oxide support (MgO, Al 2 O 3 , ZrO 2 , and CeO 2 ), and further explored its influence on the state of Cu species as well as the catalytic performance in CO 2 hydrogenation to methanol. The results show that the introduction of Nd 3 + can effectively induce lattice distortion of the support which promotes the generation of oxygen vacancies and the formation of surface basic sites, thereby enhancing the interfacial electronic interaction between Cu and support and improving the stability of Cu + active centers. Among them, the Cu catalyst supported on Nd-doped ZrO 2 exhibited the best catalytic performance such as the high CO 2 conversion and selectivity to methanol. Various characterization (XRD, SEM, in-situ XPS, H 2 -TPR, CO 2 -TPD, and H 2 -TPD) results confirmed the key role of Nd-doping in regulating the oxygen defects, electronic structure, and Cu species distribution over support. This study reveals the structural regulation mechanism of Nd in constructing efficient Cu-based catalysts for CO 2 hydrogenation from the perspective of support engineering, providing theoretical basis and practical guidance for the design of new high-performance catalytic materials.
✓ 已验证
产品关联
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2022
·
IF 4.831
Kaixiang Ji,Fangshuo Liu,Tesfaye Hailemariam Barkae,Shuai Quan,Abdallah M. Zeid,Wei Zhang,Jianping Li,Guobao Xu
N -hydroxyphthalimide (NHPI) is an efficient organic catalyst and an important chemical raw material which can be used as an intermediate in organic synthesis of drugs and pesticides. In this study, NHPI has been used as a coreactant of lucigenin chemiluminescence (CL) for the first time. The CL of the developed system is significantly enhanced in the presence of Co 2+ . Therefore, we developed a novel lucigenin-NHPI CL method coupled with flow injection analysis for the sensitive, precise, and selective determination of Co 2+ . The linear range of this method is 1–1000 nM, and the detection limit is 67 pM (S/N = 3). In addition, this method has a good selectivity for Co 2+ . It has been applied to the detection of Co 2+ in lake water, and the standard recovery rate is 95.9–103.2%, indicating that the method is feasible.
研究领域:
分析化学
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环境科学
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化工
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Anqi Jiao,Yiran Zhang,Lin Yang,Xuteng Zhao,Chunping Wu,Ting Chen,Reggie Zhan,Zhen Huang,He Lin
Measuring the CO 2 concentration is the base of carbon accounting which aims to abate the greenhouse gas emission. This paper pays attention to developing sensitive material for CO 2 detection in vehicle exhaust. For this purpose, La 1-x FeO 3-δ nanoparticles with A-site deficiency were synthesized by flame spray pyrolysis (FSP). The dynamic response of the prototype CO 2 sensors was evaluated by checking the gas-mixture with 5%–15% CO 2 . It was observed that the amount of A-site deficiency would obviously affect the performance of the material. La 0.95 FeO 3-δ sensor exhibits the highest response (S = 3.38) and a relatively short response time (t 90 = 114s) among the serial La 1-x FeO 3-δ sensors (x = 0, 0.02, 0.05, 0.07 and 0.1). The improvement of the response might be attributed to the increase of oxygen vacancies and the higher valence of B-site cations caused by the introduction of A-site deficiency. Furthermore, the sensor exhibited good selectivity against NH 3 , NO, NO 2 and CO, as well as good repeatability. However, water vapor is still a disturbance in the response. The response at 40% RH and 80% RH are 2.11 and 1.73, respectively. Finally, the sensing mechanism based on the participation of the oxygen vacancies was discussed.
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
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Chenxuanzi Wang,Mingxuan Zhong,Yongcheng Cai,Zewei Zhang,Bo Xiao,Tingting Xu,Xun Wang
The chemical looping reforming coupled with CO 2 splitting (CLR-CS) offers a promising solution for syngas production and simultaneous decomposition of CO 2 . In this study, the Sr-Fe based oxygen carriers (OCs) were evaluated in CLR-CS using ethanol as fuel. The presence of Sr significantly improved the oxidation performance of iron oxides. The Sr element in fresh Sr-Fe based OCs mainly formed two crystal phases, including SrFe 12 O 19 and Sr 4 Fe 6 O 13 . Increasing the amount of Sr element made it easier to form Sr 4 Fe 6 O 13 crystal phase. The Sr 4 Fe 6 O 13 was favorable for syngas production, due to the higher surface oxygen vacancy formation energy with a range of 3.13–3.37 eV. However, the lower oxygen transfer capacity (OTC) of Sr 4 Fe 6 O 13 resulted in a lower CO yield in the of stage of CO 2 decomposition. Compared with Sr 4 Fe 6 O 13 , SrFe 12 O 19 exhibited the higher OTC and the higher reactivity of lattice oxygen, which was preferable to produce more CO 2 in the stage of ethanol reforming in fuel reactor. During the cycle tests, the crystalline phase of SrFe 12 O 19 didn’t regenerate under the CO 2 atmosphere but transformed into Sr 4 Fe 6 O 13 . It was attributed to the lower energy barrier of CO 2 oxidation on the oxygen defect surface of Sr 4 Fe 6 O 13 . The phase transformation of SrFe 12 O 19 accompanied the formation of Fe 3 O 4 . The excessive Fe 3 O 4 had poor stability and inactivated easily due to sintering and agglomeration in Sr1Fe4 and Sr1Fe6 samples. The Sr1Fe2, namely the molar ratio of SrO to Fe 2 O 3 of 1:2, exhibited the better performance for syngas (0.291 Nm 3 /kg OC) and CO (0.141 Nm 3 /kg OC) coproduction at 800 °C. Additionally, the Sr1Fe2 presented an excellent cyclic stability in 30 cycles due to the suitable proportion of Sr 4 Fe 6 O 13 and iron oxides formed, which maintained a high syngas yield and avoided sintering of iron oxides. Overall, the Sr1Fe2 is a promising OC candidate in CLR-CS process.
研究领域:
能源科学
·
材料科学
✓ 已验证
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Zhang Qian,Lu Wei,Wu Mingyue,Qi Guansheng,He Zhenglong,Li Jinliang
To solve the environmental problems caused by greenhouse gas emissions, a type of oxidized nanocellulose (NC)@chitosan (CS)@silica sol (Sol) gel foam based on electrostatic interactions was obtained by simple blending and freeze drying. The self-assembly process was driven by electrostatic forces between the negatively charged NC and Sol and positively charged CS. The gas adsorption properties of the gel foams under various ratios of constituents were studied by orthogonal experiments. The gel foam had a good adsorption capacity for CO 2 at 30 °C. After eight adsorption–desorption cycles, the adsorption efficiency remained above 90%, indicating that the gel foam structure was stable. Infrared (IR) and X-ray photoelectron spectroscopy (XPS) analyses showed that CO 2 adsorption occurred via physical adsorption. The interaction state and adsorption mechanism of CO 2 and gel foam adsorption were explained using a molecular dynamics model. In addition, the gel material can be used as a filling material in underground coal mines for low-temperature resistance and to prevent the spontaneous combustion of coal. This conforms to the concept of sustainable development and has significant theoretical research significance.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
Science Advances
·
2021
·Vol. 7
·期 47
·
IF 14.143
Zhong Liang,Lianpeng Song,Mingzi Sun,Bolong Huang,Yaping Du
Electrochemical reduction of CO 2 (CO 2 RR) to value-added liquid fuels is a highly appealing solution for carbon-neutral recycling, especially to syngas (CO/H 2 ). Current strategies suffer from poor faradaic efficiency (FE), selectivity, and controllability to the ratio of products. In this work, we have synthesized a series of single and dual atomic catalysts on the carbon nitride nanosheets. Adjusting the ratio of La and Zn atomic sites produces syngas with a wide range of CO/H 2 ratios. Moreover, the ZnLa-1/CN electrocatalyst generates the syngas with a ratio of CO/H 2 = 0.5 at a wide potential range, and the total FE of CO2RR reaches 80% with good stability. Density functional theory calculations have confirmed that the Zn and La affect electronic structures and determine the formation of CO and H 2 , respectively. This work indicates a promising strategy in the development of atomic catalysts for more controllable CO 2 RR.
研究领域:
电化学
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催化
·
材料科学
·
环境科学
·
能量转换
✓ 已验证
DOI
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2022
·
IF 6.364
Jing-Hui Zhang,Fang-Ze Han,Cheng-Xin Li,Shan-Lin Zhang
Recently, SrTi 0.3 Fe 0.7 O 3−δ (STF) has been investigated as a highly stable oxygen electrode material for solid oxide electrochemical cells (SOCs) with a sufficiently low resistance for cell operation at temperatures of > 700 °C. However, in general, the STF electrode performance is limited at temperatures of ≤ 700 °C due to the low oxygen surface exchange coefficient, which is mainly caused by high Sr surface segregation. To improve the electrode performance, Sr 0.9 (Ti 0.3 Fe 0.7 )O 3−δ (A-STF) with an A-site-deficient design is developed to reduce the Sr content and thus reduce the Sr surface segregation, thereby providing a unique combination of excellent oxygen electrode performance and long-term stability. The A-site deficiency reduces the electrode polarization resistance by > 3 times at 600 °C and clearly improves the oxygen diffusion and surface exchange coefficients due to the decrease of Sr surface segregation. The A-STF electrode exhibits stable performance in the fuel cell and electrolysis modes at 1 A cm −2 > 1200 h. The stability of STF-based oxygen electrodes in a CO 2 -enriched atmosphere is investigated, and the results indicate that A-STF exhibits excellent CO 2 tolerance.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
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