Journal of Experimental Nanoscience
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2021
·
IF 3.075
Ying Zhang,Yangmei Li,Qiang Tan,Song Hong,Zhenyu Sun
Electrochemical CO2 reduction (ECR) powered by renewable electricity is reckoned to provide an effective strategy to alleviate environmental issues and energy crisis, enabling a potential carbon neutral economy. To boost the ECR to fuels and value-added chemicals, the design of highly active and selective catalysts is important. In this study, we demonstrate facile ultrasonication-facilitated synthesis of two-dimensional copper terephthalate for efficient ECR. High faradaic efficiencies (FEs) of up to 72.9% for hydrocarbons are achieved at a mild overpotential in an H-type cell. In particular, the FE for ethylene (C2H4) formation approaches 50.0% at an applied potential of −1.1 V (vs. the reversible hydrogen electrode), outperforming commercial Cu, Cu2O, CuO, Cu(OH)2 and many recently reported Cu-based materials. The C2H4 partial geometric current density is as high as ∼6.0 mA·cm−2. This work offers a simple avenue to developing advanced electrocatalysts for converting CO2 into high-value hydrocarbons.
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Fundamental Research
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2021
·
IF 0
Yannan Zhou,Pengfei Yan,Suoying Zhang,Yunxiao Zhang,Hongwei Chang,Xiaoli Zheng,Jingyun Jiang,Qun Xu
Combining the physical advantages of two-dimensional (2D) inorganic nanosheets and the modular design and programmed structure of metal-organic frameworks (MOFs), 2D MOFs remain at the forefront of functional material research. Despite tremendous efforts, precise control in the synthesis of 2D nonlayered MOFs with predesigned topology for desired applications remains challenging. Success in the bottom-up synthesis of 2D nonlayered MOFs via ligand exchange motivated us to incorporate partial BTC (BTC = 1,3,5-benzenetricarboxylate) ligand dissociation and CO 2 capped coordination into the top-down treatment of bulk Cu-BTC MOF, leading to successful conversion of a 3D nonlayered network to a 2D Cu-based topological structure. Notably, a supercritical CO 2 -containing solvent mixture is employed to provide the desired defect and coordination engineering. Thus, our work introduces a new top-down concept based on modulated synthesis to fabricate high-quality 2D nonlayered MOFs for the first time.
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Solar RRL
·
2021
·Vol. 5
·期 12
·2100703
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IF 8.582
Junxiang Xiang,Tingshi Zhang,Ruodan Cao,Mingxiong Lin,Bixia Yang,Yonglin Wen,Zanyong Zhuang,Yan Yu
In designing highly efficient CO 2 reduction reaction (CRR) photocatalysts with excellent selectivity and efficiency, a key limitation is the poor understanding on the mechanism response of the active sites of catalysts to CRR selectivity and activity. Herein, it is revealed how the concentration of point defect affects the CRR selectivity and activity of catalysts. Quasi-2D NiO nanosheets (NSs) that are composed of NiO nanoparticles (NPs), and finely tuned the oxygen vacancies (OVs) concentration of the NSs by regulating the grain size (≈5–25 nm) of NPs are created. The NiO with moderate OVs concentration has the highest photocatalytic CRR efficiency and selectivity ( V CO = 17.2 μmol h −1 , 98.3%), outperforming other prepared NiO catalysts and reported Ni-based photocatalysts. Density functional theory calculation associated with the CO 2 temperature-programmed desorption confirms that the moderate OVs concentration enables strong CO 2 binding to promote CO 2 adsorption and activation and allows efficient charge transfer. In contrast, excessive OVs reduce the CO 2 binding affinity and restrain charge mobility, both detrimental to the CRR performance.
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Chemistry-An Asian Journal
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2021
·Vol. 16
·期 20
·3141-3150
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IF 4.568
Haoyu Wang,Jing Zheng,Jing Zhao,Wanqin Jin
Graphical Metal ions are successfully incorporated into GO channels , which contribute to facilitating CO 2 transport, decreasing N 2 solubility, hindering N 2 diffusion, and form multiple interactions with GO nanosheets, thus achieving the remarkably improved CO 2 /N 2 separation performance (with separation factor increasing 12.2 times) and excellent long-term stability. Graphene oxide (GO) membranes holds great potential for high-performance CO 2 capture. Aiming at enhancing the CO 2 separation performance and structural stability of GO membranes, functionalizing GO channels with metal ions confers a promising strategy. In this study, we reported the fabrication of metal ion-incorporated GO membranes with remarkably improved CO 2 /N 2 separation performance. The metal ions within GO channels contribute to facilitating CO 2 transport, decreasing N 2 solubility, hindering N 2 diffusion, and form multiple interactions with GO nanosheets. After introducing Mg 2+ ions, the CO 2 /N 2 separation factor of GO membrane is remarkably increased from 4 to 48.8 with the CO 2 permeance increases 1.5 times. Moreover, the separation performance of the GO-Mg 2+ membranes shows an excellent long-term stability owing to the structural robustness. This study could provide insights into the regulation of the microstructure of metal ion-functionalized GO membranes for highly selective transport of specific molecules.
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PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2021
·Vol. 31
·期 38
·2105001
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IF 18.808
Yushuai Xu,Jian Han,Yidong Luo,Yaochun Liu,Junping Ding,Zhifang Zhou,Chan Liu,Mingchu Zou,Jinle Lan,Ce-wen Nan,Yuanhua Lin
Gaseous CO 2 reduction driven by solar energy is a promising solution to the current energy crisis and environmental problems. Although thermocatalysts, electrocatalysts, and photocatalysts are developed as classical strategies for CO 2 reduction, it remains a challenge for high efficiency and CO 2 net reduction during this process. Here, a multi-field driven hybrid catalyst, Pt/ZnO nanorod arrays/Bi 1-x Er x CuSeO, is designed using the photo-thermoelectric effect, which can take advantage of both photocatalysis and thermocatalysis. The results indicate that the maximum CO production rate of 2.91 µmol g −1 h −1 at 423 K can be realized in such Pt/ZnONR/Bi 0.9 Er 0.1 CuSeO hybrid catalyst, as can be ascribed to a synergetic photo-thermoelectric effect (i.e., light irradiation can provide heat, photo-excited carriers, and the concomitant Seebeck voltage). The band alignment of ZnO/BiCuSeO heterojunction and carriers transport are proposed to be optimized by the Er doped BiCuSeO thermoelectric supports, greatly enhancing the catalytic performance. The application of thermoelectric support could be promising in the structure design of multi-field driven hybrid catalysts, and such a photo-thermoelectric catalytic process demonstrates a desirable way of solar energy utilization in CO 2 transformation.
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APPLIED SURFACE SCIENCE
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2021
·
IF 6.707
Jianfei Xiao,Yuan Wang,Tian C. Zhang,Shaojun Yuan
Nitrogen-sulfur codoped porous carbon (NSPC) is a promising advanced material, showing great application potential in greenhouse gas capture and energy storage. Here, a novel NSPC with controllable porous structure was fabricated via pyrolysis and activation of N, -containing polycondensates, which were synthesized by one-pot polycondensation reaction of triglycidyl isocyanurate, glucose and thiourea. The obtained sample NSPC-1-650 showed cross-linked spherical morphology with uniform pore size (2.61 nm), large specific surface areas (1927.46 m 2 ·g −1 ), and the doping of nitrogen (4 wt%) and sulfur (2 wt%), which leaded to a good CO 2 adsorption capability (5.56 mmol·g −1 at 298.15 K, 5 bar) and excellent stability. Additionally, when used as a supercapacitor, the NSPC-1-650 sample showed an ultrahigh specific capacitance (224.3F·g −1 at 1 A·g −1 in 6 M KOH electrolyte), an excellent rate capability, and good stability (retained > 85% capacity after 5000 cycles). Notably, the all solid-state symmetrical NSPC-1-650-based supercapacitors delivered a high energy density (the maximal value = 7.8 Wh·Kg −1 ) and power density (the maximal value = 4500 W·Kg −1 ). These results suggest that NSPC-1-650 be a competitive candidate as a CO 2 adsorbent and supercapacitor.
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ChemSusChem
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2021
·Vol. 14
·期 8
·1962-1969
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IF 8.928
Yanling Qiu,Wenbin Xu,Pengfei Yao,Qiong Zheng,Huamin Zhang,Xianfeng Li
Graphical A helping hand : Copper electrodes derived from Cu 2 O with predominant (111) facets are synthesized by cetyltrimethylammonium bromide-assisted preparation. The optimized electrode shows a high faradaic efficiency of 90 % for formic acid obtained by electrochemical reduction of CO 2 at −2.0 V (vs.SCE), which surpasses most reported Cu electrodes. The electrochemical reduction of CO 2 (ERC) to valuable chemicals has attracted extensive attention. However, the relatively low selectivity and efficiency of the reaction remain challenges. In this study, Cu electrodes derived from Cu 2 O with predominant (111) facets are synthesized by cetyltrimethylammonium bromide-assisted preparation. The optimized electrode shows a high faradaic efficiency of 90 % for HCOOH obtained by ERC at −2.0 V (vs.SCE), which surpasses most reported Cu electrodes. Based on a comprehensive analysis of the relationship between the catalytic activity and the thickness of the Cu 2 O layer, the catalytic activity of the unit active site on the Cu 2 O-derived Cu electrodes is found to be higher than that on the blank Cu electrode. DFT calculations indicate that OCHO* would be produced preferentially over *COOH in the presence of cetyltrimethylammonium bromide (CTAB). This deduction is verified by testing of the effects of CTAB and KBr addition on HCOO − selectivity.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Xiaoqian Li,Dechao Wang,Zhongjie He,Fangfang Su,Nan Zhang,Yangyang Xin,Hongni Wang,Xiaolu Tian,Yaping Zheng,Dongdong Yao,Mingtao Li
Porous liquids (PLs) as a novel class of materials combine the permanent porosity of microporous solids, the rapid mass transfer of liquids, and fluidity, thus exhibiting extraordinary promise for gas capture and separation. However, the practical application of PLs was severely restricted by their undesirable relative high viscosity and melting temperature. In this work, the symmetric dicationic ionic liquids [C 6 BIm 2 ][NTf 2 ] 2 was synthesized as a steric hindrance solvent to construct a type of low viscosity zeolitic imidazolate frameworks (ZIFs)-based PLs. Specifically, the ZIF-67-PLs-2 ( i.e. , ZIF-67 loading of 2.0% in PLs) presented a low viscosity with 543.4 mPa·S at 25 °C, which was about 20 times lower than that of type III PLs reported previously. Meanwhile, ZIF-67-PLs showed long-term stability even over 180 days and broke the fluidity limitation down to −64 °C, broadening the work conditions. Moreover, ZIF-67-PLs-10 ( i.e. , ZIF-67 loading of 10.0% in PLs) achieved 55 times CO 2 and 7 times toluene adsorption capacity more than those of the corresponding pure DILs, respectively. Remarkably, the fascinating features of ZIF-67-PLs including lower viscosity, wide liquid range and higher adsorption pave a new way for the optimal design of novel PLs towards gas uptake and separation.
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Materials Today Nano
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2021
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IF 8.109
C. Zeng,K. Wang,L. Pan,B. Li,J. Li,L. Zhou,W. Zhang,C. Liang,H. Pan
Green synthesis of nanocarbons from greenhouse gas CO 2 has been achieved by introducing lithium hydride into CO 2 system. However, the role of lithium hydride in determining the morphology and microstructure of nanocarbons is not revealed. Herein, the morphology and porosity of nanocarbons are found to be related to particle sizes of LiH. Gas blowing velocities of H 2 and CO 2 , increased with the decreasing particle size of LiH, and their distribution are revealed to the most important factors for the morphology and porosity of nanocarbons. The understanding of the roles of lithium hydride in green synthesis of nanocarbons may shed light on the design and large-scale synthesis of nanomaterials with desired morphology and microstructure.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Wang Jia-Wei,Jiang Long,Huang Hai-Hua,Han Zhiji,Ouyang Gangfeng
The fulfillment of a high quantum efficiency for photocatalytic CO 2 reduction presents a key challenge, which can be overcome by developing strategies for dynamic attachment between photosensitizer and catalyst. In this context, we exploit the use of coordinate bond to connect a pyridine-appended iridium photosensitizer and molecular catalysts for CO 2 reduction, which is systematically demonstrated by 1 H nuclear magnetic resonance titration, theoretical calculations, and spectroscopic measurements. The mechanistic investigations reveal that the coordinative interaction between the photosensitizer and an unmodified cobalt phthalocyanine significantly accelerates the electron transfer and thus realizes a remarkable quantum efficiency of 10.2% ± 0.5% at 450 nm for photocatalytic CO 2 -to-CO conversion with a turn-over number of 391 ± 7 and nearly complete selectivity, over 4 times higher than a comparative system with no additional interaction (2.4%±0.2%). Moreover, the decoration of electron-donating amino groups on cobalt phthalocyanine can optimize the quantum efficiency up to 27.9% ± 0.8% at 425 nm, which is more attributable to the enhanced coordinative interaction rather than the intrinsic activity. The control experiments demonstrate that the dynamic feature of coordinative interaction is important to prevent the coordination occupancy of labile sites, also enabling the wide applicability on diverse non-noble-metal catalysts.
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PubMed
高影响因子
COMPOSITES SCIENCE AND TECHNOLOGY
·
2021
·
IF 8.528
Bozhen Wu,Fa-Qian Liu,Shu-Wen Luo,Liu-Qin Zhang,Fangxin Zou
A new three-dimensional (3-D) interconnected elastic scaffold with high thermal conductivity was prepared from hydroxylated graphene (HG) and hydroxylated carbon nanotubes (HCNTs). Then, polyethyleneimine (PEI) was uniformly covalently grafted to the surfaces of the scaffold, to give a HG-HCNTs-PEI nanocomposite as a superior CO 2 adsorbent. The resulting nanocomposites possess high amine loading (9.46 mmol N g −1 ) and high adsorption capacity in simulated flue gas (up to 4.43 mmol CO 2 g −1 ). Due to the excellent thermal conductivity (5.1 W/mK), the adsorbents exhibit superior cyclic stability even in harsh desorption temperature (135 °C), Thus, these carbonaceous materials-supported adsorbents make the CO 2 capture process practical and promising.
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ACS Sustainable Chemistry & Engineering
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2021
·
IF 8.198
Xiaochen Xu,Jie Dong,Xian Xiao,Xin Zhao,Qinghua Zhang
At present, the glassy polymeric membrane technology for CO2 separation is still confronted with a predicament that it is still difficult to fabricate membranes with both high CO2 permeance and high gas selectivity. Fortunately, newly developed thin film composite membranes (TFC) (∼100 nm) can facilitate high CO2 permeation by minimizing gas trans-membrane resistance and macrovoid defects. Herein, a novel TFC membrane containing a thin polyimide (PI) selective layer on a PDMS-modified PSf substrate was successfully constructed in situ by an interfacial cross-linking reaction between the amine-end-capped PI oligomer and the trimesoyl chloride (TMC) in a mild solvent system. The thickness of the thin PI selective layer is in the range of 103–485 nm and can be optimized by adjusting the interfacial polymerization parameters such as the TMC concentration. The resultant TFC membrane comprising a polyimide selective layer exhibits an optimum CO2 permeance of 330 GPU with the CO2/N2 and CO2/CH4 ideal selectivities of 30 and 32, respectively. It is an obvious improvement in CO2 separation performance compared with conventional PI flat membrane. In addition, these membranes also show an excellent plasticizing resistance and long-term stability attributed to the cross-linking structure and thin nature. It is expected that this TFC membrane structure combined with its facile fabricating process can facilitate the development of thin glassy polymeric membranes for CO2 separation.
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