Journal of CO2 Utilization
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2022
·
IF 8.321
Shujie Liang,Gongchang Zeng,Xiaohui Zhong,Hong Deng,Zuqi Zhong,Zhang Lin,Jianlin Huang
Photoreduction of diluted CO 2 is an effective strategy for the sustainable and environmentally friendly development of energy. In this study, lattice strain in NiSe is modulated through the control of the Ni concentration for the photoreduction of diluted CO 2 . Refined XRD data and the results of the Williamson–Hall analysis indicate that the lattice strain is induced by lattice distortion caused by an absence of Ni atoms in the crystal lattice . In pure CO 2 , the cumulative CO yield and selectivity of Ni 1−x Se nanoflowers reached approximately 19.39 µmol and 90.7 % in 3 h, respectively. For lower CO 2 concentrations of 0.1 and 0.05 atm, the CO selectivity of Ni 1−x Se was approximately 72.7 % and 61.7 %, respectively. On characterization of the synthesized nanoflowers , we deduced that the lattice-strained Ni 1−x Se exhibited a favorable electronic band structure that improved the separation efficiency of the photogenerated carriers . DFT calculations results revealed that the lattice strain significantly facilitated the adsorption and activation of CO 2 , which resulted in highly efficient CO 2 photoreduction. This study provides an effective strategy for the design and synthesis of high-performance catalysts based on the modification of their crystal structures.
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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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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Mengyang Xu,Xiaoxue Zhao,Haopeng Jiang,Songtao Chen,Pengwei Huo
Converting carbon dioxide into valuable chemicals is seen as a promising strategy for slowing global warming while enriching energy supplies. Photocatalysts derived from Metal-Organic Frameworks (MOFs) can not only overcome the problem of poor stability of MOFs, but also inherit the advantages of MOFs to some extent. Herein, carbon doped In 2 O 3 (C-In 2 O 3 ) hollow tubular is synthesized by calcination of MIL-68(In) as sacrificial template. Then C-In 2 O 3 and g-C 3 N 4 are hydrothermal to obtain C-In 2 O 3 /g-C 3 N 4 heterojunction . The unique hollow tubular structure, carbon doping and type-II heterojunction of C-In 2 O 3 /g-C 3 N 4 expand the light absorption capacity and promote the separation of photogenerated electron-hole pairs, thus significantly improve the activity of photocatalytic reduction of CO 2 . Among them, C-In 2 O 3 /g-C 3 N 4 -5 shows the highest CO 2 reduction activity towards CO (153.42 μmol/g/h) and CH 4 (110.31 μmol/g/h).
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ChemSusChem
·
2021
·Vol. 15
·期 1
·e202102010
·
IF 8.928
Han Zhang,Yu Yang,Yongxiang Liang,Jun Li,An Zhang,Han Zheng,Zhigang Geng,Fengwang Li,Jie Zeng
Graphical Lend me your EORs : Electrochemical oxidation-reduction (EOR) processing of a Cu-based metal-organic framework results in the formation of sub-nanometer Cu clusters that retains the organic linkers for highly selective and durable electrosynthesis of methane from the electrochemical CO 2 reduction reaction. Electrochemical CO 2 methanation powered by renewable electricity provides a promising approach to utilizing CO 2 in the form of a high-energy-density, clean fuel. Cu nanoclusters have been predicted by theoretical calculations to improve methane selectivity. Direct electrochemical reduction of Cu-based metal-organic frameworks (MOFs) results in large-size Cu nanoparticles which favor multi-carbon products. This study concerns an electrochemical oxidation-reduction method to prepare Cu clusters from MOFs. The derived Cu clusters exhibit a faradaic efficiency of 51.2 % for CH 4 with a partial current density of >150 mA cm −2 . High-resolution microscopy, in situ X-ray absorption spectroscopy, in situ Raman spectroscopy, and a range of ex situ spectroscopies indicate that the distinctive CH 4 selectivity is due to the sub-nanometer size of the derived materials, as well as stabilization of the clusters by residual ligands of the pristine MOF. This work offers a new insight into steering product selectivity of Cu by an electrochemical processing method.
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PubMed
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 1
·243-257
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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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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Debo He,Wenji Ruan,Jibiao Li,Jiupai Ni,Chengsheng Ni
The large-scale integration of intermittent renewable energies into the power grid could reduce the CO 2 emission from the combustion of fossil fuel, but it requires energy storage techniques to balance the energy production and demand. The electrolysis of CO 2 that converting electricity into chemicals/fuels provides a sustainable way of energy storage and CO 2 reduction. Solid oxide electrolysis cell (SOEC) operating at around 800 °C was able to provide highly efficient transformation of CO 2 because the high temperature was able to decrease the energy demand and increase the activation of CO 2 than room temperature electrolysis. In this study, Mo-doped ferrite perovskite , La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 , was studied as the cathode of an SOEC for the direct electrolysis of CO 2 at 800 °C. Cell with La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 cathode showed a significantly higher current density during CO 2 electrolysis than the one with La 0.55 Sr 0.45 FeO 3 cathode. Compared with the parent La 0.55 Sr 0.45 FeO 3 cathode that will subject to a superficial decomposition into Fe 0 and SrO or SrCO 3 at an elongated cathodic bias of − 1.4 V, Mo-doping will induce the production of Ruddlesden-Popper phase ( e.g. (La,Sr) 2 (Mo,Fe)O 4 , Fe-Mo-O oxides and Fe 0 ). La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 cathode was found to an unobvious current decrease at − 1.1 V, but a cell degradation was found under a high bias of − 1.4 V. During the 97 h’ aging under a cathodic bias (−1.4 V), the reduced molybdenum cation in La 0.55 Sr 0.45 Fe 0.85 Mo 0.15 O 3 was found to be less mobile than Fe 3+/2+ , La 3+ or Sr 2+ , and the perovskite with Fe-deficit region were also found to be important for the activation of CO 2 and dissociation of CO in the electrochemical process.
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Advanced Science
·
2021
·Vol. 9
·期 4
·2104138
·
IF 16.806
Aya Gomaa Abdelkader Mohamed,Enbo Zhou,Zipeng Zeng,Jiafang Xie,Dunfeng Gao,Yaobing Wang
Electrochemical CO 2 reduction (ECR) is one of the promising CO 2 recycling technologies sustaining the natural carbon cycle and offering more sustainable higher-energy chemicals. Zn- and Pb-based catalysts have improved formate selectivity, but they suffer from relatively low current activities considering the competitive CO selectivity on Zn. Here, lead-doped zinc (Zn(Pb)) electrocatalyst is optimized to efficiently reduce CO 2 to formate, while CO evolution selectivity is largely controlled. Selective formate is detected with Faradaic efficiency (FE HCOOH ) of ≈95% at an outstanding partial current density of 47 mA cm –2 in a conventional H-Cell. Zn(Pb) is further investigated in an electrolyte-fed device achieving a superior conversion rate of ≈100 mA cm –2 representing a step closer to practical electrocatalysis. The in situ analysis demonstrates that the Pb incorporation plays a crucial role in CO suppression stem from the generation of the Pb–O–C–O–Zn structure rather than the CO-boosted Pb–O–C–Zn. Density functional theory (DFT) calculations reveal that the alloying effect tunes the adsorption energetics and consequently modifies the electronic structure of the system for an optimized asymmetric oxo-bridged intermediate. The alloying effect between Zn and Pb controls CO selectivity and achieves a superior activity for a selective CO 2 -to-formate reduction.
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Journal of CO2 Utilization
·
2021
·
IF 7.132
Jiehong He,Shaoshuai Chang,Haoran Du,Bo Jiang,Wenzhao Yu,Zhenwu Wang,Weiwei Chu,Lanfang Han,Jian Zhu,Hexing Li
The hydrogenation of carbon dioxide (CO 2 ) to formic acid (FA) has been considered as a promising approach to utilize CO 2 and realize carbon-neutral energy supply. Development of efficient heterogeneous catalysts is an interesting yet challenging task. In this work, a reliable amorphous NiRu 0.1 B catalyst was presented and displayed a sufficient catalytic activity for the hydrogenation of CO 2 into FA. The amorphous structure of catalysts provided abundant dangling bonds and unsaturated atoms for enhancement of the reactant gas adsorption. Moreover, the electron-donating effect of B element is crucial for creating active electron-rich metal centres, which is proposed to facilitate the formation of the M H for activating CO 2 molecules. Owing to synergistic effect of amorphous structure and electron-donating, amorphous NiRu 0.1 B catalysts show a higher activity and stability than that of Ni-B and crystalline Ni-B at low temperature. This work not only exhibits a facile method to prepare amorphous bimetallic catalysts, also demonstrates that amorphous metals are promising heterogeneous catalysts for the hydrogenation of CO 2 to FA.
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TRANSACTIONS OF TIANJIN UNIVERSITY
·
2021
·Vol. 27
·期 3
·269-277
·
IF 0
Shi Han,Cheng Yingying,Kang Peng
The metal oxide/nitrogen-doped carbon (NC) compounds zirconium oxide/NC (ZrO 2 /NC) and cerium oxide/NC (CeO 2 /NC) were synthesized via the pyrolysis of polyaniline on the metal oxide surface. The characterization of the ZrO 2 /NC and CeO 2 /NC catalysts showed more active CO 2 reduction reaction activity than that of NC catalyst without metal oxide. Gas chromatography analysis revealed that CO and H 2 were the primary products, and no liquid-phase products were detected via proton nuclear magnetic resonance spectroscopy or high-performance liquid chromatography. The maximum Faraday efficiency of ZrO 2 /NC reached 90% at − 0.73 V (vs. RHE), with the current density of CO at 5.5 mA/cm 2 ; this Faraday efficiency value was higher than that of NC (41%), with the current density of CO at 3.1 mA/cm 2 . The interaction between the metal oxide and carbon allowed the efficient formation of defect sites, especially imine-type nitrogen, strengthening the adsorption of the key reaction intermediate CO 2 •− and thus promoting the CO 2 reduction reaction.
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JOURNAL OF THE CHINESE CHEMICAL SOCIETY
·
2021
·Vol. 68
·期 10
·1897-1907
·
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
·
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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