Sustainable Energy & Fuels
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2021
·Vol. 5
·期 14
·3598-3605
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IF 6.367
Tangxi Chen,Min Zhou,Wen Chen,Yuyao Zhang,Siyong Ou,Yueli Liu
Halide perovskite quantum dots (HP QDs) have been widely used in the field of photocatalysis due to their excellent performance. However, the issues of lead toxicity and instability prevent their process in the photocatalysis application. Herein, the lead-free Cs2AgInCl6 perovskite quantum dots (CAIC QDs) are synthesized by the hot-injection method, and CAIC QDs@Ag composites with various Ag loading amounts are self-assembled by adjusting the Cl source in the synthesis process, which is used to improve the CO2 photoreduction efficiency by using the surface plasmon resonance (SPR) effect of Ag nanoparticles. In addition, the surface ligand density of CAIC QDs@Ag composites is regulated by the purification processing treatment to release the influence of organic ligands on the charge transport performance. It is found that the CAIC QDs@Ag composite with the optimal ligands density possesses fast electron transport and effective carrier separation efficiency, which are crucial for the improvement of the photocatalysis reaction. As a result, the CAIC QDs@Ag-2 composite after purification processing achieves the highest yield of 26.4 μmol g−1 and 28.9 μmol g−1 for CO and CH4, respectively, during the CO2 photoreduction process. In addition, there is no significant decline of CO2 photoreduction performance after the photocatalysis cycling test for 9 h, indicating the good stability of the CAIC QDs@Ag composite in the photocatalysis process.
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CARBON
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2021
·
IF 9.594
Mengyang Shu,Zhijie Zhang,Zhongliang Dong,Jiayue Xu
Converting CO 2 into valuable fossil fuels through artificial photosynthesis is regarded as an appealing approach to address the problems of global warming and energy crisis, which primarily depends on the development of robust and effective photocatalysts . Herein, we illustrate the construction and fabrication of a multiwalled carbon nanotube (MWCNT)/CsPbBr 3 perovskite quantum dots (QDs) nanocomposite with efficient CO 2 photoreduction activity. In this photocatalytic system, the highly conductive MWCNT acts as an electron acceptor to inhibit the carrier recombination in the CsPbBr 3 QDs. When the content of MWCNT was 4.0 wt%, the resultant CsPbBr 3 /MWCNT exhibited the optimum photocatalytic performance, with the yields of CO and CH 4 3.14 and 2.13 times that of pristine CsPbBr 3 QDs, respectively. The rapid electron extraction and transfer from CsPbBr 3 QDs to MWCNT, as well as the enhanced visible light harvesting ability accounted for the remarkable photocatalytic performance. This work is anticipated to provide new pathway for designing efficient perovskite-based photocatalyst in energy conversion applications.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Qingxue Liu,Yuefeng Song,Rongtan Li,Houfu Lv,Weicheng Feng,Yuxiang Shen,Xiaomin Zhang,Guoxiong Wang,Xinhe Bao
CO 2 electrolysis through solid oxide electrolysis cells (SOECs) is a promising strategy for converting CO 2 to useful fuels and chemicals powered by renewable energy. Ba 0.5 Sr 0.5 Co 0.8 Fe 0.2 O 3-δ (BSCF) is a widely-investigated anode material of SOEC on account of its high and catalytic activity . However, its poor stability under CO 2 atmosphere limits its application as cathode in CO 2 electrolysis. Herein, we develop a vanadium-doped BSCF material Ba 0.5 Sr 0.5 (Co 0.8 Fe 0.2 ) 1-x V x O 3-δ (BSCFV x ) for SOEC cathode. The doping of V into B site of BSCF decreases the basicity of perovskite oxide and increases its stability under CO 2 atmosphere, thus improving the CO 2 electrolysis performance. Compared to BSCF, the cell of BSCFV 0.01 cathode shows a better tolerance to CO 2 and achieves 48.3% increase in current density at 1.6 V and 800 °C.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2021
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IF 5.455
Meng Rong,Liangrong Yang,Chao Yang,Jiemiao Yu,Huizhou Liu
Herein, a new tetraphenyladamantane-cored triazine-based multiamine (TPADT) was designed and synthesized. Its bulky molecular volume, strong rigidity, and high amine functionality enable it easy to prop up the polymer backbone and form a high hypercrosslinking degree to obtain high microporosity. A series of highly microporous tetraphenyladamantane-based polyaminals (Ad-MALPs) were prepared through the catalyst-free copolymerization of TPADT and commercial aromatic aldehydes. By changing the strut length and functionality of aldehyde monomers , the resulting polymers exhibit tailored BET surface area (1541–1779 m 2 /g) and narrow ultramicropore size distribution (0.52–0.93 nm). Ad-MALP-2 with the largest microporosity possesses the highest CO 2 uptake (21.1 wt %, 273 K/1.0 bar) and CO 2 /N 2 adsorption selectivity (35.2). Interestingly, Ad-MALP-3 shows the highest H 2 uptake (2.26 wt%, 77 K/1.0 bar) due to larger total pore volume . In addition, highly microporous Ad-MALPs simultaneously contain aromatic and cycloaliphatic components, and thus show exceptionally large aromatic and cycloaliphatic organic vapor adsorption capacity under low pressure. At P/P 0 = 0.1, the benzene and cyclohexane vapor uptakes of Ad-MALPs are up to 44.8 wt% and 39.0 wt %, far exceeding that of most previously reported porous organic polymers . Considering that Ad-MALPs have outstanding gas adsorption performance, simple preparation, good stability, and cycle ability, they are expected to be promising adsorbent materials for CO 2 adsorption/separation, H 2 storage and low-concentration volatile organic vapors capture.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Xia Lv,Lu Huang,Siyuan Ding,Jiangnan Wang,Long Li,Chao Liang,Xueqin Li
In this work, a novel dual-facilitated bio-inspired zeolitic imidazolate framework (Bio-ZIF) was proposed to simulate the structure and function of carbonic anhydrase (CA), because it can overcome the low stability and high price of the CA. A novel type of mixed matrix membrane (MMM)-composed of Bio-ZIF and Pebax® MH 1657 (Pebax) was fabricated and used to enhance CO 2 separation performance. The bio-inspired active sites of Bio-ZIF can catalyze the reversible hydration of CO 2 in the form of bicarbonate to facilitate the quick transport of CO 2 across the MMMs, increasing CO 2 permeability. Furthermore, the amino groups of Bio-ZIF reacted with CO 2 to produce zwitterion as an intermediate during the reversible reaction, facilitating CO 2 permeation in the MMMs. It can be concluded that Bio-ZIF performed the dual-facilitated functions in the MMMs by reversible hydration and reversible reaction with CO 2 molecules. Thus, the as-prepared MMMs exhibited an excellent CO 2 separation performance. Particularly, Pebax/Bio-ZIF-12 MMM presented an optimal CO 2 permselectivity with CO 2 permeability of 542 ± 6.0 Barrer and CO 2 /CH 4 separation factor of 40 ± 0.4, surpassing the 2008 upper bound. This work provided an ingenious strategy to design bio-inspired fillers to achieve dual-facilitated functions in MMMs for enhancing CO 2 separation.
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Molecular Catalysis
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2021
·
IF 5.062
Tianqinji Qi,Weizuo Li,Hong Li,Ke Ji,Shaoyun Chen,Yongchun Zhang
Revealing the origin of the enhanced performance on yttria (Y 2 O 3 ) promoted Cu/ZnO based catalyst for methanol synthesis via CO 2 hydrogenation is still challenging. To shed light upon the promotion effect of Y 2 O 3 modifier on binary Cu/ZnO catalyst for CO 2 hydrogenation reaction, a ternary Cu/ZnO/Y 2 O 3 catalyst was synthesized via a citric acid coordination-assisted strategy. The developed Cu/ZnO/Y 2 O 3 catalyst exhibited a remarkably higher Weight-time yeild of methanol (236.8 g MeOH g cat −1 ∙ h − 1 ) and methanol selectivity (81.1%) in comparison to Cu/ZnO catalyst (159.6 g MeOH g cat −1 ∙ h − 1 and 73.9%, respectively). Various characterizations results have uncovered the enhanced catalytic activity of Cu/ZnO/Y 2 O 3 catalyst for methanol synthesis was associated with small size and highly dispersed Cu species and abundant surface adsorption sites as well as more Cu-ZnO interfaces with strong interaction. Moreover, the Cu/ZnO/Y 2 O 3 catalyst displayed a superior weight-time yield of methanol with a time-on-stream of 100 h in comparison with classic Cu/ZnO catalyst. We anticipate that this basic design strategy will provide a novel alternative to expand opportunities to explore scalable, cost-effective catalysts for industrial methanol synthesis.
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Tingting Zhai,Caihong Wang,Fengjuan Gu,Zi-hui Meng,Wenfang Liu,Yanzi Wang
Enzymatic conversion of CO2 to high-value chemicals is a green route of resource reutilization, which is limited by low solubility of CO2 in mild conditions. Here, silica microspheres were first modified by the co-deposition of polyethyleneimine (PEI) and dopamine and the resultant polydopamine (PDA)/PEI-SiO2 was then used as the strengthening material of the enzymatic conversion of CO2 to formate. The initial reaction rate increased from 13.4 to 27.2 times with the loading amount of PDA/PEI-SiO2 increasing from 0.1 to 0.4 g. Following that, PDA/PEI-SiO2 was used as the carrier for the immobilization of carbonic anhydrase (CA). As a result of synergism, the formate synthesis was accelerated up to 48.6 times with a low loading amount of 0.2 g of PDA/PEI-SiO2-CA. Although the promoting effect of PDA/PEI-SiO2 retained only 56.1% after being used once, PDA/PEI-SiO2-CA retained 95.1% activity after 10 cycles of use. It was presumed that CA boosted the impact and reusability of PDA/PEI-SiO2 by improving CO2 desorption. This work is much significant in providing a simple and high-efficiency strategy for process intensification of enzymatic CO2 conversion.
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ACS Applied Materials & Interfaces
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2020
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IF 8.758
Yunlei Shi,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Hucheng Zhang,Jianji Wang
In recent years, metal–organic frameworks (MOFs) have been explored as emulsifiers for the fabrication of Pickering emulsions and then used for hybrid material synthesis and interface catalysis. Nevertheless, stimuli-responsive Pickering emulsions stabilized by MOFs have been rarely reported so far, although they are of great importance for fundamental research studies and practical applications. Herein, for the first time, triethylenetetramine (TETA)-functionalized MOFs (ZIF-90/TETA) have been designed, synthesized, and used for fabricating CO2-/N2-response Pickering emulsions. It is shown that even at the ZIF-90/TETA content of 0.25 wt %, the functional MOF can still efficiently emulsify n-hexane and water to form a high internal phase Pickering emulsion. Importantly, the Pickering emulsion can be easily and reversibly switched between emulsification and demulsification by bubbling of CO2 and N2 alternatively at atmospheric pressure. The possible mechanism of the CO2/N2 switchable emulsion is investigated by zeta potential, water contact angle, interfacial tension, 13C NMR spectroscopy, and an optical microscope. It is found that the acid–base reaction of CO2 with TETA anchored on the surface of ZIF-90 leads to the production of hydrophilic ammonium bicarbonate and carbamate, which results in the emulsification of the Pickering emulsion. However, when N2 is bubbled to remove CO2, the reverse reaction takes place to cause the demulsification of the Pickering emulsion. Moreover, the CO2/N2 switchable Pickering emulsion has been successfully used as a microreactor for Knoevenagel reactions to demonstrate a highly efficient integration of chemical reaction, product separation, and ZIF-90/TETA recycling for a sustainable chemical process.
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PubMed
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
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IF 4.65
Jianfei Xiao,Yuan Wang,Tian C. Zhang,Shaojun Yuan
A novel porous carbon derived from glucose and dicyandiamide incorporated with reduced graphene oxide (rGO) was prepared for CO 2 capture and supercapacitors . In this synthesis, one-pot hydrothermal and KOH activation were employed to obtain reducing graphene oxide/N-doped porous carbon (rGO/NPC) composites. Among the rGO/NPC composites derived, the sorbent rGO/NPC-600-2-1 (1 represents the addition amount of graphene oxide is 1% of the total mass of glucose and dicyandiamide, 2 represents the mass ratio of potassium hydroxide to the precursor of carbon composite material is 2 and 600 means activation temperature is 600 °C) had a large surface area of 865.1 m 2 g −1 , a rich nitrogen doping amount of 7.07 wt%, and a high CO 2 capture ability of 5.77 mmol/g at 298 K. Additionally, the as-synthesized rGO/NPC-600-2-1 was used as a supercapacitor electrode, providing a specific capacitance 210.8 F g −1 in 6 M KOH electrolyte under ambient conditions and excellent charge and discharge long cycle stability (circa 100% capacitance retention at a current density of 10 A g −1 after 10000 cycles). Even at a high current density of 20 A g −1 , a capacity of 141.1 F g -1 is still maintained. The results above suggested that the rGO/NPC composites are applicable candidates for both electrochemical energy storage and CO 2 capture.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Yamei Huang,Peiyao Du,Wen-Xiong Shi,Ye Wang,Shuang Yao,Zhi-Ming Zhang,Tong-Bu Lu,Xiaoquan Lu
Solar-driven CO 2 reduction with H 2 O oxidation into liquid fuels is highly desirable for sustainable carbon cycle to achieve carbon neutral, but represents a great challenge for artificial photosynthesis. Herein, bimetallic PdIn nanoclusters are confined in a photosensitizing covalent organic framework (N 3 -COF) to facilely construct Pd x In y @N 3 -COF composites (x:y = 1:0, 0:1, 1:2, 1:1, 2:1). The resulting PdIn@N 3 -COF exhibits excellent activity for CO 2 photoreduction with H 2 O oxidation as the H + and e − source, showing a record-high total yield of 798 μmol g -1 for producing CH 3 OH (74 %) and CH 3 CH 2 OH (26 %) among the framework materials. The synergy in both the bimetallic nanocluster and cluster@N 3 -COF contributes greatly to C C coupling and interfacial charge transfer, thus achieving excellent activity for conversion of CO 2 to C 1 /C 2 alcohols on the non-copper catalysts. This work highlights the amazing potential for constructing bimetallic nanocluster@photosensitizing supports to produce alcohols in artificial photosynthesis with H 2 O oxidation.
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Journal of Energy Chemistry
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2021
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IF 9.676
Rui Yang,Zipeng Zeng,Zhen Peng,Jiafang Xie,Yiyin Huang,Yaobing Wang
Currently most of research efforts for selective electrocatalysis CO 2 reduction to C2+ products have relied on crystalline Cu-based catalysts; amorphous Cu with abundant low-coordinated atoms holds greater promise for this conversion yet remains relatively underexplored. Here we report an amorphous urchin-like Cu@nanosilica hybrid synthesized by electrostatic coupling Si polyanions with Cu salt in hydrothermal processes. The Cu@nanosilica electrocatalyst displays excellent CO 2 electroreduction activity and selectivity with a Faradic efficiency of 70.5% for C2+ product production, and higher stability compared to the crystalline Cu counterpart. The solar-driven CO 2 electrolysis yields an energy efficiency of 20% for C2+ product production. Mechanism study reveals that the urchin-like Cu@nanosilica catalyst with amorphous Cu/Cu + dispersion enhances CO 2 adsorption and activation to facilitate generation of CO 2 − * and possible CO* intermediates, and suppresses hydrogen evolution concurrently. The combined effects of both aspects promote efficient C2+ product production from CO 2 electroreduction.
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
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2021
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IF 2.262
Yi Zhao,Yangchuan Ke,Xu Hu,Fangfang Peng,Chengcheng Yu,Liang Xing
A new kind of CO2 responsive polymeric surfactant (named DEA-SSS) was synthesized by using 2-(diethylamino)ethyl methacrylate (DEA) and sodium styrene sulfonate (SSS) via radical polymerization. The structure and composition of the copolymer were characterized by FT-IR spectrometer, 1HNMR, and elemental analyzer. It was found that the surface and interfacial tension would be much reduced by adding the synthesized surfactant at low concentration. The amphiphilic copolymer could be dispersed in water after bubbling CO2 and precipitated out upon N2 injection. The variation of copolymer solution with and without CO2 adding was also characterized by electric conductivity meter and transmission electron microscopy (TEM). Pickering emulsion of liquid paraffin in water was prepared using the copolymer as the sole emulsifier with high speed stirring. It was demulsified after purging with CO2 and emulsified again by removal of CO2. The nano-emulsion was made using method of phase inversion composition at elevated temperature through mixing the surfactant with Brij30. When the CO2/N2 were bubbled circularly, the size distribution of nano-emulsions would change reversibly.
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