Catalysis Science & Technology
·
2021
·Vol. 11
·期 23
·7727-7739
·
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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Ke Chen,Linhan Ni,Hao Zhang,Jia Xie,Xin Yan,Saisai Chen,Junwen Qi,Chaohai Wang,Xiuyun Sun,Jiansheng Li
The interfacial compatibility between fillers and polymers essentially influences the separation performance of mixed matrix membranes (MMMs). In this work, an one-pot synthesized functional layer veiled zeolite imidazolate frameworks-67 (VZIF-67) was used as an efficient nanofillers to fabricate MMMs via physical blending with 6FDA-Durene polyimide. Benefiting from the CO 2 affinity from functional layer and the intrinsic characteristics of porous nanofillers, significant enhancement on separation performance was observed on the resultant MMMs. Specifically, the optimized VZIF-67 MMMs (30 wt% loading) exhibited CO 2 /CH 4 selectivity of 32.5 with CO 2 permeability of 1210 Barrer, which is 1.7 and 1.5 times higher than those of the control membrane, respectively. More importantly, the surface organic attribute and abundant amine groups of VZIF-67 reinforced the interfacial compatibility between the nanofillers and polymer matrix, leading to a doubled CO 2 /CH 4 selectivity compared with the ZIF-67 MMMs. Overall, the performance of the VZIF-67 membrane toward CO 2 /CH 4 separation surpasses the 2008-updated Robeson upper bound. These results indicate the functionalization strategy on porous nanofillers is a promising approach to fabrication of high performance of MMMs.
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DALTON TRANSACTIONS
·
2021
·Vol. 51
·期 2
·541-552
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IF 4.39
Dong Fang,Linlin Zhang,Yongjian Niu,Yuanyuan Wang,Qingxiao Su,Jiao Wang,Cheng Wang
SnO2 is one of the most promising catalysts for CO2 electroreduction. However, the intrinsic low electrical conductivity and weak CO2 adsorption and activation capability have rendered the reaction kinetically sluggish and inefficient. To surmount these hurdles, herein, W was incorporated into SnO2 nanosheets to modulate the electronic structures. Compared with pristine SnO2, the p-band centre of W-doped SnO2 was elevated towards the Fermi level, accompanied by the reduction in the band gap and work function. As a result, both the CO2 adsorption and the electron transfer process were promoted, thus lowering the activation energy barrier for CO2 reduction. Benefitting from these, a maximum faradaic efficiency of 87.8% was achieved for HCOOH at −0.9 V vs. the RHE. Meanwhile, the current density and energy efficiency approached 20.92 mA cm−2 and 60%, respectively. Such performances could sustain for 14 h without obvious fading and exceeded pristine SnO2 and most reported Sn-based catalysts. Tafel slope and reaction order analyses further suggested that the reaction proceeded following a stepwise electron–proton transfer pathway with the formation of CO2˙− as the rate determining step. This work demonstrated the effectiveness of electronic structure tuning in promoting the catalytic performances of p-block metal oxides and contributed to the development of efficient catalysts for sustainable energy conversion and carbon neutrality.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Xiaoqin Shi,Shufeng Shen
Nonaqueous secondary alkanolamine-based systems, replacing conventional water with 2-alkoxyethanols as cosolvents, have recently attracted much attention for an energy-efficient CO 2 capture process. In this work, physical solubility of N 2 O and CO 2 in 2-(methylamino)ethanol (MAE), 2-methoxyethanol (2-ME) and their blends was measured and correlated at temperatures ranging from (283.2 to 333.2) K. Vapor-liquid equilibrium (VLE) data for the CO 2 + MAE + 2-ME system at 7.8, 19.4 and 39.1 mass% MAE were also measured in a stirred equilibrium cell at temperatures of (313.2–393.2) K and CO 2 partial pressures up to 270 kPa. VLE data were represented by a modified Kent-Eisenberg model with an AARD of 12.6%. The apparent equilibrium constants considering the liquid nonideality were well correlated as a function of temperature, concentration of carbamate product and CO 2 loading.
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Journal of CO2 Utilization
·
2021
·
IF 7.132
Zhongzheng Zhang,Shijian Lu,Guofei Shen,Yonghui Zhao,Tianyang Zhu,Qiang Gao,Nannan Sun,Wei Wei
The rapid synthesis of highly ordered nitrogen-doped mesoporous carbon single crystals with regular and tunable single-crystal morphologies were successfully realized via a controllable co-assembly strategy by using F127 as structure-directing template, 2-methylimidazole as nitrogen source and morphology-adjusting agent, and hexamethylenetetramine as formaldehyde source. Compared with other methods for carbon crystal growth, intricate pre-polymerization steps, taxing synthesis conditions, and long duration time are not requisite for this strategy. Detailed investigation on the effects of 2-methylimidazole dosage, hydrothermal temperature and time, and carbonization temperature on morphology, structure, and nitrogen content of carbon crystals were systematically conducted. Furthermore, one reasonable assembly mechanism was elucidated from both experimental and theoretical perspectives. It was found 2-methylimidazole actively involved in the formation of the polymer matrices via H-bonding to surfactant and chemical reactions with formaldehyde and resorcinol. As such, the introduced 2-methylimidazole not only acted as an effective nitrogen precursor to significantly promote the nitrogen content in resulted crystal carbons, but also served as a positive morphology-tuning agent. Its increasing use successfully achieved the morphology adjustment from hexagonal prisms to rhombic dodecahedrons and then spheres. With intrinsic enriched nitrogen content and large surface area, our synthesized carbon crystals show excellent CO 2 adsorption performance.
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Membranes
·
2021
·Vol. 12
·期 1
·8
·
IF 4.106
Yunzhao Guo,Wenbo Qi,Kaiyun Fu,Xianfu Chen,Minghui Qiu,Yiqun Fan
Ceramic membrane contactors hold great promise for CO2desorption due to their high mass transfer area as well as the favorable characteristics of ceramic materials to resist harsh operating conditions. In this work, a hydrophobic tubular asymmetric alpha-alumina (α-Al2O3) membrane was prepared by grafting a hexadecyltrimethoxysilane ethanol solution. The hydrophobicity and permeability of the membrane were evaluated in terms of water contact angle and nitrogen (N2) flux. The hydrophobic membrane had a water contact angle of ~132° and N2flux of 0.967 × 10−5mol/(m2∙s∙Pa). CO2desorption from the aqueous monoethanolamine (MEA) solution was conducted through the hydrophobic tubular ceramic membrane contactor. The effects of operating conditions, such as CO2loading, liquid flow rate, liquid temperature and permeate side pressure, on CO2desorption flux were investigated. Moreover, the stability of the membrane was evaluated after the immersion of the ceramic membrane in an MEA solution at 373 K for 30 days. It was found that the hydrophobic α-Al2O3membrane had good stability for CO2desorption from the MEA solution, resulting in a <10% reduction of N2flux compared to the membrane without MEA immersion.Keywords:membrane contactor;carbon dioxide;desorption;ceramic membrane
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Mu Liu,Xiaolei Bao,Fahao Ma,Minrui Wang,Liren Zheng,Zeyan Wang,Peng Wang,Yuanyuan Liu,Hefeng Cheng,Ying Dai,Yuchen Fan,Zhaoke Zheng,Baibiao Huang
Enhanced photocatalytic performance and excellent stability are usually regarded contradictory during photocatalytic reaction. In this study, supercycle ALD was employed to achieve superior performance and stability simultaneously for the system of TiO 2 @Cu during CO 2 reduction reaction, which was unattainable by post-deposition TiO 2 , a commonly-employed technique for enhancing stability. More oxygen vacancy, partially-covered Cu species as well as well-maintained charge separation capability of alternatively-deposited TiO 2 @(2Cu + 2TiO 2 ) × 25 could be the reason for enhanced activity and stability as suggested by a series of characterizations such as Single-particle TRPL and Single-particle PL. Experimental data also suggested unselective and mixed-layer deposition of TiO 2 and Cu loaded in the mode of alternative-deposition. The method proved in our study could be applicable in synthesizing other ALD-prepared catalysts with enhanced performance and stability, which will be a big step forward towards comprehensively utilizing the potential of ALD technique in the field of photocatalysis.
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RSC Advances
·
2021
·Vol. 11
·期 46
·28535-28541
·
IF 3.361
Peng Wang,Mingzhi Wang,Jianqiao Lu
Direct conversion of CO2 to high value-added carbon products based on molten salt electrochemistry has been proven to be a feasible approach to solve the climate problem and achieve carbon neutrality. In this work, carbon nanotubes (CNTs), carbon spheres (CSs) and honeycomb carbon are synthesized by electrolysis of a single or multiple alkali metal carbonate electrolyte. The elemental composition, morphology and structure, crystallinity and graphitization degree of carbon products are characterized by electron dispersive spectroscopy (EDS), scanning electron microscopy (SEM), transmission electron microscope (TEM), X-ray diffraction (XRD) and Raman microspectroscopy (RAM). The results demonstrate that a high yield of CNTs is obtained in Li2CO3 electrolyte by regulating the electrolysis temperature and current density. Compared to pure Li2CO3, Li–Na carbonate electrolyte with 1 wt% stannic oxide/cerium oxide (SnO2/GeO2) favors CS formation rather than CNT formation. Additionally, honeycomb carbon products are generated in Li–Na–K electrolyte, when the electrolysis temperature is lower than 600 °C. Overall, this work provides a novel carbon neutral strategy where high value-added carbon products are synthesized using CO2 as a carbon source.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Wenshuang Lou,Luwei Peng,Ruinan He,Yuyu Liu,Jinli Qiao
Electrochemical reduction of CO 2 to fuels and chemicals is an effective way to reduce greenhouse gas emissions and alleviate the energy crisis, but the highly active catalysts necessary for this reaction under mild conditions are still rare. In this work, we grew CuBi bimetallic catalysts on derived copper foam substrates by co-electrodeposition, and then investigated the correlation between co-electrodeposition potential and electrochemical performance in CO 2 -to-formate conversion. Results showed that the bimetallic catalyst formed at a low potential of − 0.6 V vs. AgCl/Ag electrode achieved the highest formate Faradaic efficiency (FE formate ) of 94.4% and a current density of 38.5 mA/cm 2 at a low potential of − 0.97 V vs. reversible hydrogen electrode (RHE). Moreover, a continuous-flow membrane electrode assembly reactor also enabled the catalyst to show better performance (a FE formate of 98.3% at 56.6 mA/cm 2 ) than a traditional H-type reaction cell. This work highlights the vital impact of co-electrodeposition potential on catalyst performance and provides a basis for the modulated growth of bimetallic catalysts on substrates. It also shows the possibility of preparing Bi-based catalysts with no obvious decrease in catalytic activity that have been partially replaced with more economic copper.
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CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Yingchao Hu,Hongyuan Lu,Hailong Li
Li 4 SiO 4 stands out among various solid sorbents for CO 2 capture. The commonly used mechanical granulation process for Li 4 SiO 4 sorbents causes the destruction of the microstructures. Therefore, with the characteristics of huge production and low cost, an agricultural waste (rice husk) was employed as a pore former to improve the structures of Li 4 SiO 4 pellets and, thus, enhance the cyclic CO 2 sorption performance. The rice husk templating greatly enhanced the CO 2 sorption capacity of Li 4 SiO 4 pellets. Especially, 20 wt% rice husk-templated Li 4 SiO 4 exhibited the capacity of 0.21 g/g, which was nearly twice that of the unmodified sorbent. The quick release of the combustion gases from burning rice husk could create porosity for the sorbents. In addition, the alkaline compositions in rice husk promoted the CO 2 sorption due to the decreased CO 2 diffusion resistance by the formation of molten phases. Moreover, the ashes of rice husk after high-temperature combustion were found to block the pores of the sorbents, leading to the capacity reduction. The comprehensive function of rice husk templating for Li 4 SiO 4 pellets was the tradeoff between the positive effects of pore creation and alkaline doping and the negative effects of pore blockage by the ashes.
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Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 2
·881-890
·
IF 12.732
Peng Hu,Hao Liu,Hao Wang,Jie Zhou,Yongqing Wang,Hongbing Ji
CO2 capture, especially under ultralow-pressure regions (400–10 000 ppm), is extremely essential and challenging to keep the prolonged manual operation in confined spaces and reduce CO2 corrosion in natural gas. Although many MOFs have been covered for CO2 capture, they usually suffered from unheeded morphology engineering associated with diffusion kinetics and unbridgeable CO2 adsorption under ultralow pressure. Herein, we have successfully targeted pyrazine-functionalized Co-MOF (1a′) nanocrystals having dapper hexahedral morphology through skillfully integrating morphology engineering and pore functionality. The yielded 1a′ paradigm with snug pore microenvironment afforded record-high adsorption performance for trace CO2 capture (1.36 mmol g−1 at 400 ppm and 5.7 mmol g−1 at 10 000 ppm), yet eclipsed adsorption behavior for CH4 and N2 at 298 K. The decent pore geometry awarded 1a′ with superior property for CO2/CH4 and CO2/N2 separation, giving higher IAST selectivity (1454 for 15/85 CO2/N2 and 494 for 50/50 CO2/CH4). Besides, 1a′ showed an improved hydrophobic nature, with a desired CO2/H2O uptake ratio of 0.45 and improved diffusion selectivity (DM,CO2/DM,H2O) of 17.7. Breakthrough tests visualized that 1a′ could realize high-purity CO2 (>96%), yielding maximum CO2 productivity (162 and 164.9 litres per kilogram for 18/85 CO2/N2 and 50/50 CO2/CH4). Modeling simulations have cooperatively revealed the structure–property relationship between guest molecules and the framework. This work presents an advanced benchmark adsorbent for low-concentration CO2 capture from flue gas and natural gas.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Bi,Ling Zhang,Hao Jiang,Chunzhong Li,Yanjie Hu
The precise regulation of the nano-catalyst structure is a big challenge that limits the application of photocatalytic technology in CO 2 reduction. Herein, to improve the utilization of sunlight, the separation and transfer efficiency of photogenerated electron-hole pairs, and the surface catalytic reaction process, CuInS 2 /C/TiO 2 (CIS/C/T) hierarchical tandem heterostructure have been rationally designed. Multiple in-situ characterizations and DFT simulations show that CQDs not only act as a co-catalyst, but also act as a bridge between TiO 2 (T) and CuInS 2 (CIS), which further attribute to the efficient separation and enrichment of photogenerated electron-hole pairs while effectively avoiding the recombination. In consideration of the excellent broad-spectrum absorption, the CO 2 -to-CO photoreduction performance of the optimal CIS/C/T reaches up to 7.73 μmol g -1 h −1 , about 3.16 times enhancement of C/T. Combined with in-situ DRIFTs, the intrinsic structure–activity relationship is pointed out, and extended to other similar TiO 2 -based catalytic systems (In 2 S 3 /C/TiO 2 ). This work will provide a new universal strategy for the design and synthesis of high-performance nano-photocatalysts.
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