JOURNAL OF CATALYSIS
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2021
·
IF 7.92
Huiyuan Cheng,Xuemei Wu,Xiangcun Li,Yayun Zhang,Manman Feng,Zihao Fan,Gaohong He
Electrochemical CO 2 conversion offers a sustainable approach to alleviate the energy crisis but remains a long-standing challenge. Herein, atomically dispersed FeN 5 sites anchored on N-doped carbon matrix templated by zeolitic imidazole framework-8 (ZIF-8) are facilely synthesized for efficient catalyzing CO 2 reduction. The FeN 5 single-atom catalyst (Fe-SA/ZIF) presents the Faradaic efficiency of 98% at −0.7 V vs . RHE and over 95% in a wide potential range from −0.4 to −1.0 V vs . RHE, surpassing most of the reported single-atom catalysts for CO 2 RR. Further density functional theory (DFT) calculations reveal that the outstanding activity of FeN 5 sites mainly originates from the lowered d -band center modulated by the out-of-plane coordinated pyridinic N, which reduces the CO adsorption energy from −1.71 to −1.49 eV compared to FeN 4 moieties. Thus, the synergistic effect between FeN 4 sites and the coordinated pyridine offers new insight in designing outstanding electrocatalysts for multiple applications.
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高影响因子
ACS Applied Energy Materials
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2020
·
IF 4.473
Yuanxing Wang,Cailing Niu,Yachuan Zhu,Da He,Weixin Huang
Producing syngas from electrochemical reduction of CO2 by renewable energy offers an opportunity to reduce CO2 emissions and provide chemicals and fuels. Herein, we report the careful manipulation of the reduction treatment to synthesize copper nanowire arrays (Cu NAs). By thermal oxidation, copper oxide nanowires were grown on a Cu mesh. Then, thermal reduction and electrochemical reduction were used to reduce copper oxide to Cu with the morphologic features largely preserved. The derived Cu NAs are cost-effective electrocatalysts capable of reducing CO2 and H2O for tunable syngas production. It is demonstrated that syngas, the mixture of H2 and CO, could be attained with a wide range of compositions (from 1:2 to 3:1) from CO2 reduction and H2O reduction on these Cu NAs in aqueous solutions. In addition, Cu NAs show a high current density, 4 mA/cm2, at a low potential, −0.5 V, with a high syngas faradaic efficiency of over 70%. This approach explores a new method that sheds light on tuning the syngas composition from the electrochemical CO2 reduction by Cu-based catalysts.
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JOURNAL OF POWER SOURCES
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2020
·
IF 8.247
Zhijie Wang,Tengfei Li,Qihao Wang,Anxiang Guan,Na Cao,Abdullah M. Al-Enizi,Lijuan Zhang,Linping Qian,Gengfeng Zheng
Silver-containing material is one of the efficient electrocatalysts in converting CO 2 into CO , but competing hydrogen evolution reaction (HER) in aqueous solutions results in poor energy efficiency. Here, Ag 3 subnanoclusters with the structure sensitive to CO 2 activation are in situ prepared by the cyclohexene oxidation . Hydrophobically modified Ag nanomaterials with an average particle size from 1.0 to 3.3 nm are water-repulsive, organic-soluble, and composited of the Ag 3 cluster units, possessing the electron donation and strong chemical adsorption of CO 2 . In the electroreduction of CO 2 , a high mass activity about 10,200 A cm −2 g Ag −1 is achieved for CO production at −1.4 V vs. reverse hydrogen electrode (RHE) on Ag nanoclusters with the external size of 1.9 nm, exhibiting 20 times higher than commercial Ag nanoparticles (diameters of 60–120 nm). Electrochemical tests in flow cells show an excellent mass activity of 55,000 A cm −2 g Ag −1 with a large current density of around 30 mA cm −2 for the CO production at −0.71 V vs. RHE, much higher than the previously reported Ag catalysts. Hydrophobically made Ag 3 subnanoclusters facilitate the CO 2 electroreduction to CO in aqueous solutions through accelerating the electron donation and suppressing the side reaction of water reduction.
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Sustainable Energy & Fuels
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2020
·Vol. 5
·期 4
·1026-1033
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IF 5.503
Chaokun Yang,Yanglin Chen,Ye Qu,Jiaxu Zhang,Jianmin Sun
A catalyst with activity comparable with homogeneous catalysts and easy separation like heterogeneous catalysts would be attractive for CO2 cycloaddition. Here, a series of polymerized bis-imidazolium based ionic liquids (PBIL-m) were synthesized and could act as homogeneous catalysts during the CO2 cycloaddition to epoxide process. They could be separated as heterogeneous catalysts after the cycloaddition reaction. PBIL-m was highly active for the cycloaddition reaction due to functional groups such as the imidazole ring, amino group and Br−. Specifically, the solid–liquid transition behavior endowed the PBIL-m with comparable activity to its homogeneous monomer catalysts (BIL-m). Among these PBIL-m catalysts, poly(1-vinyl imidazole-3-hexyl-1-imidazole-3-aminopropyl)dibromide (PBIL-3) exhibited superior catalytic performance due to the appropriate bridge chain compared with other PBIL-m. Under the conditions of 80 °C, 1.0 MPa and 24 h, 99% propylene carbonate yield and 99% selectivity were obtained. The PBIL-3 also showed excellent universality and recyclability. A reasonable reaction mechanism was deduced that the imidazole ring, amino group and Br− promoted the cycloaddition reaction under metal-, solvent-, and cocatalyst-free conditions. Therefore, the polymerized bis-imidazolium based ionic liquid with solid–liquid transition behavior is a promising candidate for smooth catalysis of CO2 conversion and utilization.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Shujie Liang,Xiaohui Zhong,Zuqi Zhong,Bin Han,Weiyi Chen,Kainan Song,Hong Deng,Zhang Lin
The development of biomimetic catalysis for efficient photoreduction of CO 2 is an effective alternative to address energy problems. However, amelioration on the construction of biomimetic catalysts for elevated photocatalytic performance is still challenging and demanded. Herein, a bioinspired artificial photosynthesis system is constructed based on ZrO 2 nanoframes (ZFs) and metalloporphyrin to mimic the morphology of trees. The robust backbone of the framework and the bio-inspiring porphyrins anchored on the surface of ZFs function as the strong trunk and well-ordered leaves of a tree, respectively. The biomimetic system achieves an evolution yield of 35.3 μmol during 3 h reaction with 93.1% CO selectivity and 1.84% CO apparent quantum efficiency ( A.Q.E. ), which is about 60.8 times larger than that of pure porphyrin (Ni) (0.58 μmol). Detailed analysis reveals that the catalytic system could not only achieve fast separation of the photogenerated carriers and effective CO 2 activation but also possess suitable energy levels, which could efficiently transfer electrons to the Ni catalytic sites to improve the photocatalytic activity. Furthermore, the good recycling tests could be explained by the robust supporting of frameworks as well as the strong binding of the Zr atoms and carboxyl groups of porphyrins. This work presents a simple model of biomimetic catalysts and outlines possible strategies for other biomimetic manufactures.
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CATALYSIS COMMUNICATIONS
·
2020
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IF 3.612
Yan Yu,Shuqi Li,Lu Huang,Jie Yu,Haiyan Zhang,Shuang Song,Tao Zeng
We herein reported the first case of successfully synthesizing homologous Ti(IV) − based metal−organic frameworks (MOFs) junction, comprising NH 2 -MIL-125 core and NTU-9 layer, via a MOF-on-MOF strategy. Benefiting from the core-shell structural advantages and the homophase type II junction effect, the obtained NH 2 -MIL-125@NTU-9 hybrids exhibit accelerated reaction kinetics and enhanced electron transfer behaviour in the solar-driven CO 2 reduction. The quantum efficiency of formate production at 430 nm (0.67%) and product selectivity (94.47%) over NH 2 -MIL-125@NTU-9 far surpass those of the pure NH 2 -MIL-125 (0.13%, 88.56%) and NTU-9 (0.16%, 89.26%), which is among the highest performances of MOFs reported previously.
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APPLIED CLAY SCIENCE
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2020
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IF 4.605
Xidong Du,Wenfeng Guang,Yugang Cheng,Zhenkun Hou,Zhenjian Liu,Hong Yin,Liang Huo,Ruide Lei,Couxian Shu
The greater adsorption ability of shale to CO 2 offers an alternative method to enhance shale gas recovery, where a potential solution for CO 2 sequestration into a deep shale reservoir can also be realized. Clay minerals are the important storage space for shale gas . In this work, the isotherm adsorption curves of CH 4 and CO 2 on montmorillonite at 288 K, 308 K and 328 K were obtained using gravimetric apparatus. The selectivity factor of CO 2 over CH 4 ( S CO2/CH4 ) and Henry's constants ( K H ) of CH 4 and CO 2 were calculated. More importantly, the thermodynamics parameters of CH 4 and CO 2 , including Gibbs free energy change (Δ G ), surface potential ( Ω ), isosteric heat of adsorption ( Q st ) and entropy change (Δ S ), were thoroughly analysed. The results indicate that all S CO2/CH4 values are obviously greater than one, and injecting CO 2 into a clay-rich shale reservoir to enhance the shale gas recovery is feasible. CH 4 has smaller K H than CO 2 , which shows that CH 4 has a weaker affinity on the montmorillonite surface. Low temperature helps to enlarge K H and promote the adsorption of CH 4 and CO 2 . Increasing the pressure causes the increase in Δ G and Ω of CH 4 and CO 2 . The higher Δ G and Ω of CO 2 compared to CH 4 reveal that the CO 2 adsorption on montmorillonite is more favourable and spontaneous. When the loading increases, the Q st values of CH 4 and CO 2 reduce. CH 4 has a smaller Q st than CO 2 , which suggests the stronger interaction of CO 2 with montmorillonite. CH 4 and CO 2 have decreasing Δ S with the loading. Under larger surface coverage conditions, the disorder of the adsorbed molecules is larger, and most of the injected molecules are trapped as a free state in the pore space . The higher ΔS of CO 2 illustrates that CO 2 molecules constitute a much more stable rearrangement than CH 4 molecules. The temperature has a slight effect on the Δ S of CH 4 and CO 2 .
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ADVANCED MATERIALS
·
2020
·Vol. 32
·期 24
·2000014
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IF 27.398
Kai Feng,Shenghua Wang,Dake Zhang,Lu Wang,Yingying Yu,Kun Feng,Zhao Li,Zhijie Zhu,Chaoran Li,Mujin Cai,Zhiyi Wu,Ning Kong,Binhang Yan,Jun Zhong,Xiaohong Zhang,Geoffrey A. Ozin,Le He
The efficiency of heterogeneous photocatalysis for converting solar to chemical energy is low on a per photon basis mainly because of the difficulty of capturing and utilizing light across the entire solar spectral wavelength range. This challenge is addressed herein with a plasmonic superstructure, fashioned as an array of nanoscale needles comprising cobalt nanocrystals assembled within a sheath of porous silica grown on a fluorine tin oxide substrate. This plasmonic superstructure can strongly absorb sunlight through different mechanisms including enhanced plasmonic excitation by the hybridization of Co nanoparticles in close proximity, as well as inter- and intra-band transitions. With nearly 100% sunlight harvesting ability, it drives the photothermal hydrogenation of carbon dioxide with a 20-fold rate increase from the silica-supported cobalt catalyst. The present work bridges the gap between strong light-absorbing plasmonic superstructures with photothermal CO 2 catalysis toward the complete utilization of the solar energy.
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PubMed
高影响因子
Journal of Energy Chemistry
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2020
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IF 7.216
Yang Li,Jing Wang,Sisi Fan,Fanan Wang,Zheng Shen,Hongmin Duan,Jinming Xu,Yanqiang Huang
Synthesis of spherical carbon beads with effective CO 2 capture capability is highly desirable for large scale application of CO 2 sorption, but remains challenging. Herein, a facile and efficient strategy to prepare nitrogen-doped hierarchically porous carbon spheres was developed via co-pyrolyzation of poly(vinylidene chloride) and melamine in alginate gel beads. In this approach, melamine not only serves as the nitrogen precursor, but also acts as a template for the macropores structures. The nitrogen contents in the hierarchically porous carbon spheres reach a high level, ranging from 11.8 wt% to 14.7 wt%, as the melamine amount increases. Owing to the enriched nitrogen functionalities and the special hierarchical porous structure, the carbon spheres exhibit an outstanding CO 2 capture performance, with the dynamic capacity of as much as about 7 wt% and a separation factor about 49 at 25 °C in a gas mixture of CO 2 /N 2 (0.5:99.5, v/v).
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Hong Yan,Lei Zhao,Yinge Bai,Fangfang Li,Haifeng Dong,Hui Wang,Xiangping Zhang,Shaojuan Zeng
Carbon dioxide (CO2) is a detrimental greenhouse gas to the environment as the main contributor to global warming. However, the development of efficient methods for CO2 absorption and separation is still a great challenge. Ionic liquids (ILs) have emerged as promising solvents for CO2 separation due to negligible vapor pressure and adjustable structures. In this work, a new strategy that three superbase ILs are designed as hydrogen bond acceptor (HBA) and further combined with ethylene glycol (EG) as hydrogen bond donor (HBD) to form novel IL-based deep eutectic solvents (DESs) was proposed for efficient and reversible absorption of CO2. The results indicated that both excellent recyclability and high CO2 mass capacity up to 0.141 g CO2/g DES under 40 °C and 100 kPa are achieved by [HDBU][Im]/EG with the mass ratio of 7:3, and the value is much higher than those of most of the reported IL-based DESs. The superior CO2 absorption and desorption performances were attributed to the synergistic interaction between both IL and EG with CO2 to form carbamate and carbonate, respectively. This work provides a feasible method for designing IL-based solvents in CO2 separation applications.
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Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 1
·243-257
·
IF 2.081
Zhang Wenfei,Zhou Qulan,Qi Ji,Li Na
Cu 2 O films were prepared using an improved solution immersion method, whereas ZnO/Cu 2 O films were prepared using an electrodeposition method. Then, the pure Cu 2 O film electrodes and ZnO/Cu 2 O film electrodes were used to reduce CO 2 to CH 3 OH. The crystal structure, morphology, particle size, and specific surface area of pure Cu 2 O films prepared under different immersion times and ZnO/Cu 2 O films prepared under different deposition times and Zn 2+ concentrations were analyzed using X-ray diffraction, scanning electron microscopy, and Brunauer–Emmett–Teller analysis. The electrolytic activity of the pure Cu 2 O film electrodes and ZnO/Cu 2 O film electrodes were studied. Under the same reaction conditions, the ZnO/Cu 2 O film electrode with the Zn 2+ concentration of 0.05 M and the deposition time of 30 min had the highest total CH 3 OH yield of 315.656 μmol/cm 2 and the fastest formation rate of 52.609 μmol/(cm 2 h), and its faradaic efficiency was 45%, which was remarkably higher than that of pure Cu 2 O film electrodes under the same reaction conditions. This study highlighted that ZnO nanoparticles had a very good promotion of electrolytic CO 2 reduction on Cu 2 O film.
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高影响因子
Processes
·
2021
·Vol. 9
·期 9
·1638
·
IF 2.847
Yonggang Ma,Xin Chen,Dehui Han,Zhe Zhao,Wenting Lu
A CO2-responsive composite of multiwall carbon nanotube (MWCNT) coated with polydopamine (PDA) and polydimethylamino-ethyl methacrylate (PDMAEMA) was prepared. The PDA was first self-polymerized on the surface of carbon nanotube. 2-bromoisobutyryl bromide (BiBB) was then immobilized by PDA and then initiated the ATRP of DMAEMA on the carbon nanotube surface. The resulting composite was characterized by Fourier-transform infrared spectroscopy (FTIR) and transmission electron microscopy (TEM). The CO2-responsive test was performed by bubbling CO2into the mixture of MWCNT-PDA-PDMAEMA composite in water. A well-dispersed solution was obtained and the UV-Vis transmittance decreased dramatically. This is attributed to the reaction between PDMAEMA and CO2. The formation of ammonium bicarbonates on the surface of carbon nanotubes leads to the separation of nanotube bundles. This process can be reversed as the removal of CO2by bubbling N2.Keywords:CO2-responsive;polymer;multiwall carbon nanotube (MWCNT);composite;ATRP
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