APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Pengyan Li,Li Liu,Weijia An,Huan Wang,Wenquan Cui
Photocatalytic CO 2 reduction is a potential way to address simultaneously environmental pollution and energy shortage. However, the difficulties of CO 2 activation and C C coupling lead to quite low conversion efficiency of CO 2 to C2 products. In this study, we constructed Cu 2 O/g-C 3 N 4 heterojunction for photocatalytic CO 2 reduction to ethanol by coupling thermal field and ionic liquids (ILs). The ethanol rate reached 0.71 mmol·g −1 ·h −1 over Cu 2 O/g-C 3 N 4 under photothermalcatalysis, which is 1.89 times that of photocatalysis and 7.05 times that of thermal catalysis. The temperature enhanced thermal motion of the radical, which promotes the formation of ethanol through the ·CH 3 dimerization. The 1-aminopropyl-3-methylimidazolium bromide ILs shows superior CO 2 reduction performance with a high current density (21.3 mA·cm −2 ) than KHCO 3 electrolyte (12.8 mA·cm −2 ). The overpotential is reduced by 0.34 V, which accelerates CO 2 reduction by reducing polarization. It is found that the ILs played a key role in suppressing H 2 O reduction and increasing ethanol yield in this photothermalcatalytic strategy.
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高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 23
·7727-7739
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IF 6.119
Biao Zhu,Qianxin Xu,Xiaoyan Bao,Dawei Lu,Hao Yin,Yumei Qin,Xing-Can Shen
The development of efficient and stable photocatalysts to solve environmental issues is essential and remains a big challenge. In this work, flower-like CoNiFe-LDH is deposited in situ on g-C3N4 nanosheets, successfully constructing a Z-scheme heterojunction CoNiFe-LDH/g-C3N4 photocatalyst for the photoreduction of CO2 and photodegradation of MB dye. The synthesized nanohybrid shows superior photocatalytic CO2 performance (42.04 μmol g−1 h−1) and fast photodegradation MB performance (0.1057 min−1). The improved photocatalytic performance was attributed to the formation of the Z-scheme heterojunction with matched energy bands, and the intimate heterojunction contact interface, which significantly enhanced the interfacial charge transfer rate and improved the separation efficiency of electron–hole pairs. Moreover, the photocatalytic mechanism was proposed based on PL, photocurrent responses, EIS, and EPR experiments. This work can shed light on further application for environmental problems of Z-scheme heterojunction photocatalysts.
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Surfaces and Interfaces
·
2021
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IF 4.837
Jianhua Ge,Bin Han,Shujie Liang,Zhongfei Liu,Yuhua Xiao,Juner Kuang,Minghui Guan,Xueming Liu
Direct photoconversion of diluted CO 2 into solar fuels has theoretically and practically become a hot research topic. However, the low yields and poor selectivity of carbonaceous products hampered by the H 2 evolution reaction is still a challenge for its practical application. Herein, we demonstrate a three-dimensional (3D) nickel borate/graphene nanoarrays (Ni-B i /G) for diluted CO 2 photoreduction with boosted activity and selectivity. In simulated flue gas with 10% CO 2 , the pristine Ni-B i displays a low activity and low CO selectivity of 41.8%, indicating its tendency of producing H 2 in diluted CO 2 . However, after growing Ni-B i nanoarrays onto graphene nanosheets , the optimized 3D Ni-B i /G exhibits a high CO selectivity of 84.9% with a CO production rate of 5.1 μmol h −1 , which is about 2 times of the blank sample. The improved performance can be attributed to the synergistic effect of the introduction of rGO and unique 3D structure, which are conducive not only to accelerate the separation of photogenerated charges, but also to enrich active sites and enhance CO 2 adsorption. This work provides fundamental guidance to the rational design of well-designed hierarchical catalysts for photoconversion of low concentration CO 2 .
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2019
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IF 3.372
Shuangqing Sun,Xiqiang Zhang,Shengxiang Feng,Hongbing Wang,Yan Wang,Jianhui Luo,Chunling Li,Songqing Hu
A novel CO 2 /N 2 switchable aqueous foam was developed using a CO 2 -responsive surfactant N,N-dimethyl-N-dodecyl amine (C 12 A) and a conventional surfactant sodium dodecyl sulfate (SDS). The performance and mechanism of this switchable foam were studied by both experiment and molecular simulation methods. Experimental results demonstrate that the foam stabilized by SDS/C 12 A surfactants has better stability and water carrying capacity than single C12A foam. The foam could be rapidly switched between stable and unstable states at ambient temperature with CO 2 or N 2 as the triggers. Simulation results shows that when CO 2 was introduced, most of SDS and C 12 A molecules aggregated in the water phase, instead of adsorbing at the air-water interface to stabilize the foam films. The strong electrostatic attraction between protonated C 12 A and SDS molecules could account for the aggregation. Due to the presence of limited surfactants located at the air-water interface after introducing CO 2 , the foam bursts quickly.
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高影响因子
FUEL
·
2019
·
IF 5.128
Yu Wu,Hong Du,Yajun Gao,Xiaoyao Liu,Tingyu Yang,Long Zhao,Xiaoqing Yue,Shuai Zhang,Jianbin Zhang
As one of the most important approaches to reduce CO 2 emission from various combustion processes, CO 2 adsorption capture is facing several many challenges, including high adsorbent cost, high energy cost, and low CO 2 selectivity. In this work, four novel silicate-based nanomaterials (SBNMs), including magnesium silicate (MgSiO 3 ), manganese silicate (MnSiO 3 ), copper silicate (CuSiO 3 ) and zirconium silicate (ZrSiO 4 ), were fabricated via hydrothermal method with SiO 3 2− extracted from coal gangue (CG) for the adsorption capture of CO 2 . Under the optimum conditions, the SiO 3 2− extraction ratio from the CG reached to 77.69%. The extracted SiO 3 2− was used to synthesize SBNMs with high surface area and high thermal stability, which were characterized with Fourier transform infrared spectroscopy, X-ray diffraction, transmission electron microscopy, and nitrogen adsorption/desorption isotherms technologies. These as-obtained SBNMs exhibited CO 2 adsorption capability of (7.82–17.93) cm 3 /g at 25 °C under 1 atm, respectively. The CO 2 adsorption data were successfully fitted with Freundlich model, and the adsorption processes were obvious chemically favored, spontaneous and exothermic according to thermodynamic parameters, including Q st , Δ G ads , Δ H ads and Δ S ads . Significantly, all SBNMs showed a excellent cycle performance and strong selectivity toward CO 2 over N 2 . The aim of this work is to provide a new method of utilization of coal gangue waste and a low-cost, and highly selective CO 2 adsorbents.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Liang Wei,Ruifeng Guo,Yunqing Tang,Jiamin Zhu,Meiyang Liu,Jianqiu Chen,Yun Xu
Three kind of pure amines which have high solubility of CO 2 were used as absorbents hardly to be recovered. A series of aqueous ethoxyacetate anion-based protic ionic liquids (PILs) with three different amine cations were designed, and physical properties including measured density and viscosity were measured. Solubility of CO 2 in the three PILs solution, 90% [DMAPAH][EOAc], 90% [DEEDAH][EOAc] and 90% [DMEDAH][EOAc], were systematic determined at the range of 303.2–333.2 K under the pressure of 1.2 bar. Impressively, the solubility of CO 2 in 90% [DMAPAH][EOAc] reached up to 2.44 mol/kg, which showed more advantage than some traditional or functional ILs. The 90% [DMAPAH][EOAc] could be reused four times. Besides, the proposed mechanism was advised. Considering the advantages of high absorption capacity, low cost, easy regeneration including fast absorption rate, we believe the three PILs solution can be recommended as alternatives to some volatile organic amines to be applied in CO 2 capture.
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高影响因子
AICHE JOURNAL
·
2019
·Vol. 66
·期 2
·e16800
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IF 3.463
Xingyu Wu,Yanxiong Ren,Guomin Sui,Guangzhe Wang,Guangshuai Xu,Leixin Yang,Yingzhen Wu,Guangwei He,Nayab Nasir,Hong Wu,Zhongyi Jiang
The implementation of high-performance membranes in large-scale CO 2 capture has the potential to significantly decrease the capture cost and reduce the environmental footprints. However, highly permeable polymers rarely have sufficient selectivity for energy-efficient carbon capture. In this study, zeolite imidazolate framework hollow nanoparticles (ZIF-HNPs) were synthesized and embedded into highly permeable polymers as versatile fillers to prepare mixed matrix membranes (MMMs). The interior hollow architecture minimizes transport resistance of gas diffusion through the fillers while its molecular-sieving shell provides high selectivity. With 28 vol% loading of ZIF-HNPs, the membrane exhibits CO 2 permeability of 7,128 Barrer and CO 2 /CH 4 selectivity of 16.4 (57.7% and 31.4% higher than these of pristine membrane), which surpass the upper bound of the state-of-the-art reported polymeric membranes. Meanwhile, we proposed a modified Maxwell model based on the hierarchical structure of the MMM to analyze the effects of cavity size and loading on gas transport behaviors within membranes.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2020
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IF 3.807
Cuizhu Ye,Xingguang Chen,Junjun Xu,Huiting Xi,Tiantian Wu,Danwen Deng,Jinsheng Zhang,Ganhui Huang
Supported by metal-organic frameworks (MOFs), a new molecular imprinted electrochemical sensor (MIES) taking nano-structure Co 2+ @Fe 3 O 4 as the support point of receptor was developed for highly sensitive detection of GA in this paper. Gold electrode was modified with Co 2+ @Fe 3 O 4 , then Co 2+ @Fe 3 O 4 /Au was soaked and compounded to Fe 3 O 4 @ZIF-67/Au. MIPs film was obtained by potentiostatic polymerization with polypyrrole as monomer and GA as template. SEM, EDS, FTIR, XRD, DPV and EIS characterizations indicate the success of the preparation of the modified electrode . By optimization, the Δ i response of MIP/Fe 3 O 4 @ZIF-67/Au was strengthened from 25.38 μA to 30.84 μA. The MIP/Fe 3 O 4 @ZIF-67/Au sensor showed a superior sensitivity with a lower LOD of 0.297pM (S/N = 3) and a wider linear range of 6–600pM for GA detection, which profits from the combination of high surface area of Co 2+ @Fe 3 O 4 and high porosity of MOFs. Because of the specificity of molecular imprinted polymers (MIPs), our sensor showed advanced selectivity and not affected by similar structure interfering substances. In addition, the stability, reproducibility and real-sample detection were also satisfactory with the recovery rates between 89.5% and 118.4% and the RSD were lower than 5.5%. This sensitive and simple method can be further used to prepare polypyrrole-based MIES suported by MOFs-Co 2+ @Fe 3 O 4 for highly sensitive detection of other small and weight molecules.
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高影响因子
JOURNAL OF CATALYSIS
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2019
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IF 7.723
Shunan Zhang,Xiaofang Liu,Zilong Shao,Hui Wang,Yuhan Sun
Direct CO 2 hydrogenation to ethanol is one of the promising and emerging routes for the transformation of CO 2 into value-added chemicals, but it remains a major challenge because of low ethanol selectivity and catalytic stability. In this work, Na-promoted cobalt catalysts supported on different materials (Al 2 O 3 , ZnO, AC, TiO 2 , SiO 2 , and Si 3 N 4 ) were evaluated to elucidate the effects of supports. The SiO 2 - and Si 3 N 4 -supported catalysts exhibited efficient generation of ethanol with 18% CO 2 conversion and 62% selectivity in the alcohol distribution at 250 °C, whereas CH 4 was predominantly produced on other supported catalysts. Characterization results indicated that the Co 2 C active phase only remained intact on SiO 2 and Si 3 N 4 supports during reaction and exhibited excellent durability for 300 h, which was attributed to the existence of a strong metal–support interaction (SMSI) obtained by Si O Co bond formation. In situ DRIFTS results revealed that CO produced on Co 2 C inserted into CH x intermediates to form ethanol. Moreover, CO as the reactive intermediate could induce the regeneration and reconstruction of decomposed Co 2 C on the surface for catalytic sustainability.
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JOURNAL OF MEMBRANE SCIENCE
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2019
·
IF 7.015
Yutao Liu,Hong Wu,Luofu Min,Shuqing Song,Leixin Yang,Yanxiong Ren,Yingzhen Wu,Rui Zhao,Hongjian Wang,Zhongyi Jiang
2D material membranes with well-defined interlayer nanochannels hold great promise for precise molecular separation, where the size and surface chemical property of the channel determine the separation efficiency. The currently reported 2D material membranes for efficient CO 2 separation are primarily built by introducing crosslinkers or intercalators into the interlayer channel. In this study, we demonstrate a novel 2D material membrane with inherent CO 2 -selective transport channels based on layered double hydroxide (LDH). The intrinsic breathing effect of LDH toward CO 2 enables the spontaneous incorporation of CO 2 molecules into the interlayer nanochannels and subsequent conversion/transport in the form of CO 3 2− species which are released as CO 2 at the downstream side of membrane. Moreover, the intercalated CO 3 2− ions with an ionic radius of 0.136 nm narrow down the nanochannel size from 0.7 nm to 0.3 nm by electrostatic interaction with LDH layers, conferring the membrane a distinct molecular sieving ability for CO 2 /CH 4 separation. The unique breathing effect and size-sieving effect jointly contribute to the high membrane separation performance with CO 2 permeance of 150 GPU and CO 2 /CH 4 selectivity of 33. This study is anticipated to extend the materials and strategies for design of the CO 2 preferential transport channels in membranes.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Min Wang,Nicholas Preston,Nengneng Xu,Yanan Wei,Yuyu Liu,Jinli Qiao
The electrochemical reduction of CO2 at ambient conditions provides a latent solution of turning waste greenhouse gases into commodity chemicals or fuels; however, a satisfactory ion-conducting membrane for maximizing the performance of a CO2 electrolyzer has not been developed. Here, we report the synthesis of a sequence of hydroxide-conductive polymer membranes, which are based on polymer composites of poly(vinyl alcohol)/Guar hydroxypropyltrimonium chloride, for use in CO2 electrolysis. The effect of different membrane functional groups, including thiophene, hydroxybenzyl, and dimethyloctanal, on the efficiency and selectivity of CO2 electroreduction to formate is thoroughly evaluated. The membrane incorporating thiophene groups exhibits the highest Faradaic efficiency of 71.5% at an applied potential of −1.64 V versus saturated calomel electrode (SCE) for formate. In comparison, membranes containing hydroxybenzyl and dimethyloctanal groups produced lower efficiencies of 67.6 and 68.6%, respectively, whereas the commercial Nafion 212 membrane was only 57.6% efficient. The improved efficiency and selectivity of membranes containing thiophene groups are attributed to a significantly increased hydroxide conductivity (0.105 S cm–1), excellent physicochemical properties, and the simultaneous attenuation of formate product crossover.
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PubMed
高影响因子
REACTIVE & FUNCTIONAL POLYMERS
·
2019
·
IF 3.074
Dongdong Yao,Ting Li,Yaping Zheng,Zhilin Zhang
In this study, a novel hybrid nanofluid, composed of a composite core of poly(2-dimethylamino ethyl methacrylate) microgel and silica (PDMAEMA/SiO 2 ) and a shell of polyetheramine (M2070), was fabricated via a combination of inversed emulsion polymerization , biomimetic silicification and grafting onto approach. Firstly, PDMAEMA microgel of ca. 300-nm diameter with good dispersity was prepared in water/cyclohexane system. Subsequently, walnut kernel-structured and solid spherical PDMAEMA/SiO 2 composites were fabricated using swollen and contractive PDMAEMA microgel as catalytic template, respectively. Then 3-(2, 3-epoxypropoxy) propyl trimethoxysilane (KH560) modified M2070 was grafted on PDMAEMA/SiO 2 composites to obtain two kinds of solvent-free PDMAEMA/SiO 2 @M2070 hybrid nanofluids with core@shell structure. Finally, the CO 2 gas adsorption performance of these nanofluids was investigated under different CO 2 pressure (0.5–4.5 MPa) at 25 °C. The results indicated that nanofluid with walnut kernel-structured core showed more excellent CO 2 adsorption capacity than solid spherical one. Moreover, it still displayed good stability over ten adsorption-desorption cycles.
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