JOURNAL OF THE CHINESE CHEMICAL SOCIETY
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2021
·Vol. 68
·期 10
·1897-1907
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IF 1.967
Zhen Zhu,Yu-Teng Hwang,Hao-Chun Liang,Ren-Jang Wu
In this study, several Pd/MgO/BiVO 4 nanocomposites were prepared using the hydrothermal method and their effective photocatalyst activity for the photoreduction of CO 2 to CH 4 was investigated. The microstructure and photocatalytic behavior of the prepared photocatalysts were studied through X-ray diffraction, scanning electron microscopy, tunneling electron microscopy, X-ray photoelectron spectroscopy, ultraviolet–visible spectrophotometry, Fourier-transform infrared spectroscopy, Brunauer–Emmett–Teller specific surface area, and photoluminescence spectroscopy. CH 4 yields of 5.9 and 9.4 μmol g −1 hr −1 were obtained using BiVO 4 and 25% MgO/BiVO 4 nanocomposites, respectively. The highest production rate of CH 4 was measured as 12.8 μmol g −1 hr −1 on overloading 0.3% Pd on 25% MgO/BiVO 4 . Pd/MgO/BiVO 4 exhibited excellent CO 2 photoreduction stability with negligible loss after five consecutive cycles. Finally, a possible mechanism of CO 2 photoreduction using Pd/MgO/BiVO 4 was proposed for understanding the synergistic effects. The results of the experiment revealed that Pd/MgO/BiVO 4 can be a promising photocatalyst in solar energy conversion and storage application and can achieve excellent CO 2 photoreduction performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Guixian Deng,Guifang Zhang,Xing Zhu,Qingjie Guo,Xiangbiao Liao,Xi Chen,Kongzhai Li
Reduction of CO 2 in presence of oxidative impurity ( e.g. , O 2 ) is more promising than utilization of pure CO 2 due to skyrocketing cost for purification of captured CO 2 from air or industrial exhaust gas. In this work, Ni-based catalysts are modified by CeO 2 and ZrO 2 to suppress negative effect of O 2 on reforming of CO 2 with methane, which show high CH 4 conversion (97 %) and CO 2 conversion (95 %) at 750 °C and can maintain high CO 2 conversion even with high O 2 content. The physicochemical characterizations on fresh and spent catalysts show that the interaction among Ni, CeO 2 and ZrO 2 results in well dispersion of smaller Ni particles, even after long-term testing. In situ DRIFTS results show that Ni/CeO 2 -ZrO 2 -SiO 2 catalyst shows advantage to activate CH 4 to generate active CH 3 *, promoting the formation of CO, and the CeO 2 -ZrO 2 solid solution improves the CO 2 adsorption, thereby reducing the competitive effect of CO 2 and O 2 .
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Chemical Science
·
2021
·Vol. 12
·期 11
·3937-3943
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IF 9.825
Jinghui Tu,Haihong Wu,Qingli Qian,Shitao Han,Mengen Chu,Shuaiqiang Jia,Ruting Feng,Jianxin Zhai,Mingyuan He,Buxing Han
CO2 methanation is an important reaction in CO2 valorization. Because of the high kinetic barriers, the reaction usually needs to proceed at higher temperature (>300 °C). High-efficiency CO2 methanation at low temperature (<200 °C) is an interesting topic, and only several noble metal catalysts were reported to achieve this goal. Currently, design of cheap metal catalysts that can effectively accelerate this reaction at low temperature is still a challenge. In this work, we found that the amorphous Co–Zr0.1–B–O catalyst could catalyze the reaction at above 140 °C. The activity of the catalyst at 180 °C reached 10.7 mmolCO2 gcat−1 h−1, which is comparable to or even higher than that of some noble metal catalysts under similar conditions. The Zr promoter in this work had the highest promoting factor to date among the catalysts for CO2 methanation. As far as we know, this is the first report of an amorphous transition metal catalyst that could effectively accelerate CO2 methanation. The outstanding performance of the catalyst could be ascribed to two aspects. The amorphous nature of the catalyst offered abundant surface defects and intrinsic active sites. On the other hand, the Zr promoter could enlarge the surface area of the catalyst, enrich the Co atoms on the catalyst surface, and tune the valence state of the atoms at the catalyst surface. The reaction mechanism was proposed based on the control experiments.
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PubMed
高影响因子
ACS Applied Energy Materials
·
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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CHEMICAL ENGINEERING JOURNAL
·
2021
·
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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高影响因子
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
CATALYSIS COMMUNICATIONS
·
2020
·
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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高影响因子
Sustainable Energy & Fuels
·
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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高影响因子
JOURNAL OF POWER SOURCES
·
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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ACS Sustainable Chemistry & Engineering
·
2020
·
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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高影响因子
Journal of Cleaner Production
·
2020
·
IF 7.246
Shasha Wang,Yuelong Xu,Junfeng Miao,Mengshuai Liu,Bin Ren,Lihui Zhang,Zhenfa Liu
Microporous carbon xerogels (CXs) were successfully fabricated via a facile one-pot strategy using eutectic salt mixture (KCl and ZnCl 2 ) as dual activator and catalyst. Their pore structures, morphology, and selective CO 2 adsorption behaviors were thoroughly studied by varying the contents of eutectic salt mixture. The presented CXs herein showed excellent CO 2 adsorption selectivities , and the CX-4 with optimum salt concentration (12.9%) exhibited the highest CO 2 adsorption capacity of 4.39 mmol g −1 at 273 K, which was ascribed to their special microscopic pore structure. Compared with the reported carbon materials, the optimum CX-4 exhibits a comparable or superior CO 2 adsorption performance under similar conditions, showing great potential for efficient CO 2 capture and separation from flue gas and natural gas.
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高影响因子
Journal of Energy Chemistry
·
2020
·
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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