Nano Research
·
2021
·Vol. 14
·期 8
·2831-2836
·
IF 8.897
Mou Shiyong,Li Yonghao,Yue Luchao,Liang Jie,Luo Yonglan,Liu Qian,Li Tingshuai,Lu Siyu,Asiri Abdullah M.,Xiong Xiaoli,Ma Dongwei,Sun Xuping
The advancement of cost-effective and selective electrocatalyst towards CO 2 to CO conversion is crucial for renewable energy conversion and storage, thus to achieve carbon-neutral cycle in a sustainable manner. In this communication, we report that Cu 2 Sb decorated Cu nanowire arrays on Cu foil act as a highly active and selective electrocatalyst for CO 2 to CO conversion. In CO 2 -saturated 0.1 M KHCO 3 , it achieves a high Faraday efficiency (FE) of 86.5% for CO, at −0.90 V vs. reversible hydrogen electrode (RHE). The H 2 /CO ratio is tunable from 0.08:1 to 5.9:1 by adjusting the potential. It is worth noting that HCOO − product was totally suppressed on such catalyst, compared with Sb counterpart. The improving selectivity for CO could be attributed to the bimetallic effect and nanowire arrays structure.
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ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY
·
2016
·Vol. 23
·期 1
·73-85
·
IF 1.87
Hu Hangbiao,Zhang Tao,Yuan Shaojun,Tang Shengwei
Abstract The adsorption performance of multi-walled carbon nanotubes (MWCNTs) towards CO 2 gas was enhanced by covalently grafting of phenylenediamine (PDA) via an activation-grafting process. Different loading amounts were achieved by changing the activation time and the dosage of activating agent. The so-synthesized adsorbents were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, Thermogravimetry analysis, Transmission electron microscope, Raman spectroscopy and Nitrogen adsorption–desorption analysis. The CO 2 adsorption properties were studied via static volumetric method. The results indicated that the modification process did not alter the crystal structure, whilst the quantity of defect sites and amorphous structures increased greatly. Moreover, the average pore size after functionalization increased from 9.68 to 23.80 nm. 0.59 mmol·g −1 of CO 2 were captured by aminated MWCNTs at 303.15 K and 200 kPa, while the adsorption capacity of the raw materials was only 0.17 mmol·g −1 under the same conditions. Adsorption–regeneration cycles exhibited the stability of the PDA modified MWCNTs during the prolonged cyclic operations. We found that the adsorption of CO 2 on MWCNTs belonged to physical adsorption and the adsorption behavior of CO 2 on PDA modified MWCNTs was a chemical adsorption. The effective enhancement of the CO 2 capture ability was attributed to the increased number of active sites, which offered stronger interactions with CO 2 after PDA grafting.
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Nature Communications
·
2020
·Vol. 11
·期 1
·1-9
·
IF 12.121
Wang Lingxiang,Guan Erjia,Wang Yeqing,Wang Liang,Gong Zhongmiao,Cui Yi,Meng Xiangju,Gates Bruce C.,Xiao Feng-Shou
The reaction pathways on supported catalysts can be tuned by optimizing the catalyst structures, which helps the development of efficient catalysts. Such design is particularly desired for CO 2 hydrogenation, which is characterized by complex pathways and multiple products. Here, we report an investigation of supported cobalt, which is known for its hydrocarbon production and ability to turn into a selective catalyst for methanol synthesis in CO 2 hydrogenation which exhibits good activity and stability. The crucial technique is to use the silica, acting as a support and ligand, to modify the cobalt species via Co‒O‒SiO n linkages, which favor the reactivity of spectroscopically identified *CH 3 O intermediates, that more readily undergo hydrogenation to methanol than the C‒O dissociation associated with hydrocarbon formation. Cobalt catalysts in this class offer appealing opportunities for optimizing selectivity in CO 2 hydrogenation and producing high-grade methanol. By identifying this function of silica, we provide support for rationally controlling these reaction pathways.
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PubMed
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Frontiers in Bioengineering and Biotechnology
·
2021
·
IF 5.89
Yang Ruigang,Zhu Lingyun,Li Tao,Zhu Lv-yun,Ye Zi,Zhang Dongyi
Metabolic engineering of cyanobacteria has received much attention as a sustainable strategy to convert CO2 to various longer carbon chain fuels. Pinene has become increasingly attractive since pinene dimers contain high volumetric energy and have been proposed to act as potential aircraft fuels. However, cyanobacteria cannot directly convert geranyl pyrophosphate into pinene due to the lack of endogenous pinene synthase. Herein, we integrated the gene encoding Abies grandis pinene synthase into the model cyanobacterium Synechococcus sp. PCC 7002 through homologous recombination. The genetically modified cyanobacteria achieved a pinene titer of 1.525 ± 0.l45 mg L−1 in the lab-scale tube photobioreactor with CO2 aeration. Specifically, the results showed a mixture of α- and β-pinene (∼33:67 ratio). The ratio of β-pinene in the product was significantly increased compared with that previously reported in the engineered Escherichia coli. Furthermore, we investigated the photoautotrophic growth performances of Synechococcus overlaid with different concentrations of dodecane. The work demonstrates that the engineered Synechococcus is a suitable potential platform for β-pinene production.
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PubMed
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Journal of Nano Research
·
2023
·
IF 1.7
Yong Qiang Dang,Xiang Yu Feng,Bo Ni Li,Rui Huang,Jia Jia,Jian Lan Zhang,Ya Ting Zhang
Photocatalytic CO2 reduction to solar fuel is a potential way to overcome the problem of high carbon dioxide concentrations; however, the process still faces enormous challenges, such as the low light absorption efficiency and high carrier recombination rates. This work synthesized tetraphenylporphyrin-based carbon dots (TPP-CDs) for the photocatalytic CO2 reduction to CH3OH under simulated sunlight to extend the absorption region of the CDs. The conduction band of the TPP-CDs has a sufficiently negative reduction potential to reduce CO2. TPP-CDs containing 1 wt.% TPP achieved an optimum CH3OH production rate of 173.35 μmol·gcat-1·h-1, with a remarkable 2.06-fold increase compared to pristine CDs without TPP. In this study, TPP-CDs were synthesized by changing the CD precursors to improve the utilization of visible light and apply them to the photocatalytic reduction of CO2.
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TRANSACTIONS OF TIANJIN UNIVERSITY
·
2018
·Vol. 25
·期 3
·237-244
·
IF 0
Xu Yan,Wang Fan,Hou Qingfeng,Zhao Yujun,Ding Guosheng,Xu Xingguang
In this study, we developed a strategy for using the Scoggins procedure in the synthesis of acetamidines as novel CO 2 -triggered switchable surfactants via acetimidates by effectively tuning the chemical equilibrium. The as-synthesized N ’-alkyl- N , N -diethylacetamidines exhibit excellent CO 2 /N 2 switchability and their bicarbonate salts have the ability to emulsify oil–water mixtures.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xinyi Wan,Ting Wan,Chaochao Cao,Chengchun Tang,Yanming Xue,Youguo Yan,Zhen Li,Zhizhen Ye,Xinsheng Peng
The development of highly effective and durable CO 2 separation membrane is still a challenge for the carbon capture and storage. Herein, a novel BN nanosheets supported magnetic ionic liquid membrane (BN-SMILM) is constructed by nanoconfining magnetic ionic liquid (MIL) [P 6,6,6,14 ][FeCl 4 ] to the two-dimentional (2D) nanochannels of laminated BN membrane. The 2D nanochannels provide a well support and restricted space for the MIL. The nanoconfinement effect makes the magnetic [FeCl 4 ] - anions align along the center of 2D BN nanochannels, leading to selectively accelerate the CO 2 transport. The nanoconfinement effect and CO 2 separation mechanism are further explicated by the molecular dynamic simulations. As a result, compared with the polymer supported MIL membrane, the as-prepared BN-SMILM exhibits better CO 2 separation performance, with CO 2 permeability of about 227 Barrer and CO 2 /N 2 selectivity of 90 that is above the 2008 Robeson upper-bound. The BN-SMILM also presents excellent long-term stability after 7 days operation, revealing the promising applications in CO 2 separation. This work provides a new strategy to prepare high-performance supported liquid membrane materials towards practical environmental and energy application.
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Chem Catalysis
·
2022
·
IF 0
Wenjie Wu,Yulu Yang,Yitong Wang,Tiantian Lu,Qingsong Dong,Junwei Zhao,Jingyang Niu,Qingchao Liu,Zhaomin Hao,Shuyan Song
Electrosynthesis of urea from N 2 and CO 2 molecules is of immense significance but has so far been plagued by the lack of a universal design principle to guide the search for new catalysts. Herein, as exemplified by the Cu-Bi catalyst, our findings revealed that the defective Cu-Bi catalyst could offer a maximum urea concentration of 0.45 ± 0.06 mg L −1 and the largest faradaic efficiency of 8.7% ± 1.7% at −0.4 V (versus reversible hydrogen electrode [RHE]), exhibiting outstanding activity in contrast to monometallic (Cu and Bi) and bimetallic (Cu-Bi mixture and intact Cu-Bi) catalysts. Moreover, the evidence from isotope tracing experiments, in situ Raman spectroscopy, and density functional theory (DFT) calculations suggested that it is a promising strategy for the co-reduction of N 2 and CO 2 by defective Cu-Bi catalysts, switching on a light to the application of defects in electrosynthesis of urea.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·23817-23827
·
IF 12.732
Manman Feng,Xuemei Wu,Huiyuan Cheng,Zihao Fan,Xiangcun Li,Fujun Cui,Shuai Fan,Yan Dai,Guangping Lei,Gaohong He
The diatomic catalysts (DACs) provide a new strategy for efficient catalysis of CO2 reduction reaction (CO2RR) owing to their maximum atomic utility and more flexible active sites. However, it is still challenging to precisely design heteronuclear diatomic active centers and understand the coordination mechanism of binary sites at the atomic level. Herein, a nitrogen-doped carbon matrix with precisely controlled Fe–Cu diatom sites is synthesized through a metal–organic framework. The as-obtained Fe/Cu–N–C catalyst exhibits an excellent CO faradaic efficiency (>95% over a wide potential range of −0.4 to −1.1 V vs. RHE, 99.2% at −0.8 V vs. RHE), a high turnover frequency (5047 h−1 at −1.1 V vs. RHE), and a low overpotential (50 mV), thus outperforming most reported atomically dispersed catalysts. Further density functional theory calculations indicate that the synergy between Fe–Cu diatoms causes rapid charge transfer and effectively adjusts the position of the d-band center, which reduces the energy barriers for *COOH formation and *CO desorption. This work provides a new approach for advancing universal synthesis strategies to construct heteronuclear diatomic catalysts and explore synergistic effects.
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Nano Research
·
2020
·Vol. 14
·期 3
·730-737
·
IF 8.183
Chen Weiyi,Liu Xueming,Han Bin,Liang Shujie,Deng Hong,Lin Zhang
Converting carbon dioxide (CO 2 ) to diverse value-added products through photocatalysis can validly alleviate the critical issues of greenhouse effect and energy shortages simultaneously. In particular, based on practical considerations, exploring novel catalysts to achieve efficient photoreduction of diluted CO 2 is necessary and urgent. However, this process is extremely challenging owing to the disturbance of competitive adsorption at low CO 2 concentration. Herein, we delicately synthesize oxygen vacancy-laden NiO nanoplatelets (r-NiO) via calcination under Ar protection to reduce diluted CO 2 through visible light irradiation (> 400 nm) assisted by a Ru-based photosensitizer. Benefitting from the strongly CO 2 adsorption energy of oxygen vacancies, which was confirmed by density functional calculations, the r-NiO catalysts exhibit higher activity and selectivity (6.28 × 10 3 µmol·h − 1·g −1 ; 82.11%) for diluted CO 2 -to-CO conversion than that of the normal NiO (3.94 × 10 3 µmol·h −1 ·g −1 ; 65.26%). Besides, the presence of oxygen vacancies can also promote the separation of electron-hole pairs. Our research demonstrates that oxygen vacancies could act as promising candidates for photocatalytic CO 2 reduction, offering fundamental guidance for the actual photoreduction of diluted CO 2 in the future.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Kewei Liu,Zichen Zheng,Jinyong Xu,Chao Zhang
Aimed at the bottleneck problem in conventional gas sensors that the effective detection of CO 2 gas can only be accomplished at concentrations above thousands of ppm and higher operating temperature, in this work, microstructured ZnSnO 3 equipped with rambutan-like hexahedral features with the hollow interior was successfully synthesized through a facile one-step hydrothermal method. Visible light was utilized as an excitation source to further enhance the sensing property. The investigation elaborated that at optimum hydrothermal time of 16 h, ZnSnO 3 showed a high gas response (~4.65), repeatability, and long-term stability towards 400 ppm CO 2 at room temperature. The response under purple light was 3.5 times higher than that under dark conditions, resulting from photoelectrons' generation. Furthermore, ZnSnO 3 sensor had excellent selectivity to 50 ppm CO 2 . The large specific surface area and abundant oxygen vacancies of ZnSnO 3 contribute to the excellent gas-sensing performance, which addresses the dilemma that it is difficult to break through the energy barrier through surface interaction to impact the band structure and carrier concentration because CO 2 is a non-polar molecule formed by polar bonds. Therefore, ZnSnO 3 is a promising material for the development of devices utilized in medical respiratory detection, agricultural crop growth detection and other fields.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2019
·Vol. 30
·期 8
·7950-7962
·
IF 2.195
Hu Bingbing,Guo Qiang,Wang Kang,Wang Xitao
In this paper, a series of indium oxides were prepared by calcining the In(OH) 3 precursors, which were synthesized by hydrothermal method using the mixed solution of ethylenediamine (En) and water as a solvent. The morphologies, particle sizes, pore structure, crystallinity and surface defect concentration of these photocatalysts were adjusted by varying the ratio of En to water during the preparation of In(OH) 3 precursors. The results revealed that In 2 O 3 photocatalysts obtained from the precursor prepared in En containing solvent exhibited much higher photocatalytic activities for CO 2 reduction with H 2 O when compared to that derived from the precursor prepared in pure water. This result can be ascribed to several reasons as following. Firstly, the En addition with a suitable amount can improve the crystallinity of In 2 O 3 and decrease the surface defect concentration, which obviously depressed the recombination of photogenerated electrons and holes. Also, the addition of En during the preparation of precursor can decrease the particle size, increase specific surface area and pore structure, resulting into the increase of active sites. Finally, the band gap of In 2 O 3 can be slightly narrowed after the addition of En, resulting in enhanced light absorption in the visible region. When the ratio of ethylenediamine to water is 1:1, the as-prepared In 2 O 3 possessing the largest specific surface area and pore volume, enhanced light absorption ability and higher hole–electron separation efficiency, exhibited the highest photocatalytic activity. Under visible light irradiation, the H 2 , CO and CH 4 production rates of 5.3, 8.3 and 27.2 µmol/g cat /h can be achieved, respectively.
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