SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Xianhang Jin,Jiawei Fang,Qian Ma,Rong Wang,Weidong Zhang
As China pledges that its carbon emissions will peak before 2030 and that it will be carbon neutral by 2060, the CO 2 capture technology with high efficiency and low energy-consumption was expected in industry. CO 2 phase change absorbents, CPCAs, had shown a potential to reduce energy consumption for CO 2 capture. Although a lot of CPCAs were reported in the last decade, it still suffered from the lack of theoretical guidance for development. The effect of amine structure, which mainly affects cosolvent effect of amine and salting-out effect of formed salts, on developing CPCAs by means of cosolvent effect was clarified. For cosolvent effect of amine, 12 amines with various carbon chain lengths, isomers and substituents were determined by thermodynamical method and the log P of amine were proposed to characterize the cosolvent effect. The amine with long carbon chain and steric effect showed a high ability to act as a cosolvent to enhance the solubility of 1-butanol in H 2 O. The salting-out effect of formed salts by reacting amine and CO 2 was related to p K a of amine. The absorbent comprising amine with low log P and high p K a was prefer to exhibit phase separation behavior, and benefit to develop CPCAs. Based on this guideline, all amines in this study could be developed as CPCAs by adjusting kinds of amine and diluent. Moreover, to explore the absorption-desorption performance of developed CPCAs, DEA/1-butanol/H 2 O was used as example, the volume ratio, species distributions and CO 2 cyclic capacity were measured. When the absorption temperature was 303 K and desorption temperature was 373 K, The maximum CO 2 cyclic capacity of CPCA was 2.03 mol CO 2 ·kg −1 , which was 34.4% higher than that of 30 wt% DEA/H 2 O.
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ACS Nano
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2022
·
IF 18.027
Ting Wang,Liang Chen,Cong Chen,Mengtian Huang,Youju Huang,Shoujie Liu,Benxia Li
Photocatalytic CO2 conversion into a high-value-added C2 product is a highly challenging task because of insufficient electron deliverability and sluggish C–C coupling kinetics. Engineering catalytic interfaces in photocatalysts provides a promising approach to manipulate photoinduced charge carriers and create multiple catalytic sites for boosting the generation of C2 product from CO2 reduction. Herein, a Cuδ+/CeO2-TiO2 photocatalyst that contains atomically dispersed Cuδ+ sites anchored on the CeO2-TiO2 heterostructures consisting of highly dispersed CeO2 nanoparticles on porous TiO2 is designedly constructed by the pyrolytic transformation of a Cu2+-Ce3+/MIL-125-NH2 precursor. In the designed photocatalyst, TiO2 acts as a light-harvesting material for generating electron–hole pairs that are efficiently separated by CeO2-TiO2 interfaces, and the Cu–Ce dual active sites synergistically facilitate the generation and dimerization of *CO intermediates, thus lowering the energy barrier of C–C coupling. As a consequence, the Cuδ+/CeO2-TiO2 photocatalyst exhibits a production rate of 4.51 μmol–1·gcat–1·h–1 and 73.9% selectivity in terms of electron utilization for CO2 to C2H4 conversion under simulated sunlight, with H2O as hydrogen source and hole scavenger. The photocatalytic mechanism is revealed by operando spectroscopic methods as well as theoretical calculations. This study displays the rational construction of heterogeneous photocatalysts for boosting CO2 conversion and emphasizes the synergistic effect of multiple active sites in enhancing the selectivity of C2 product.
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INORGANIC CHEMISTRY
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2022
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IF 5.436
Jingsheng Zhou,Beibei An,Zhiyong Zhu,Li Wang,Jinglai Zhang
Doping heteroatoms in carbon materials is a promising method to prepare the robust electrocatalysts for the carbon dioxide reduction reaction (CO2RR), which is beneficial for sustainable energy storage and environmental remediation. However, the obscure recognition of active sites is the obstacle for further development of high-efficiency electrocatalysts, especially for the N,P-codoped carbon materials. Herein, a series of N,P-codoped carbon materials (CNP) is prepared with different N and P contents to explore the relationship between the N/P configuration and the CO2RR activity. As compared with the N-doped carbon materials, the additional P doping is helpful to improve the activity. The optimum N,P-codoped carbon materials (CNP-900) achieve 80.8% CO Faradaic efficiency (FECO) at a mild overpotential of 0.44 V. On the basis of the X-ray photoelectron spectroscopy results, the suitable ratio between pyridinic N and graphitic N and the least P–N content are beneficial for CO2RR. The density functional theory calculations further illustrate that two elementary steps to form *COOH and *CO in CO2RR are determined by the graphitic N and pyridinic N configurations, respectively. The existence of the P–N configuration breaks the equilibrium between graphitic N and pyridinic N to suppress the activity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Tingting Wei,Liyang Wang,Kaihui Mao,Jian Chen,Jun Dai,Zhiyong Zhang,Lizhe Liu,Xinglong Wu
Rapid recombination of photogenerated carriers severely impairs the performance of photocatalysts , while polarization is an effective driving force for increasing the charge separation and hence improving the photocatalytic activity . In this work, a series of magnetoelectric-coupled layered metal–organic framework (MOF) catalysts with different Co-doped contents (denoted as Ni-MOF and Co x Ni 1-x -MOF) are fabricated with different polarities and employed as novel photocatalysts for CO 2 photocatalytic reduction reaction. Our experiments show that the highest charge separation efficiency occurs in the Co 0.1 Ni 0.9 -MOF sample which has a maximal polarization. This Co 0.1 Ni 0.9 -MOF material has a best CO 2 reduction performance of 38.74 μmol g −1 h −1 which is at a high level in the currently reported layered materials. Meanwhile, it is found that a series of Co x Ni 1-x -MOF samples all display selectivity close to 100% for CO 2 reduction to CO, which is desirable for industrial applications. Theoretical analysis shows that Co doping alters the degree of distortion of the asymmetrical Ni-centered octahedron {NiN 2 O 4 } in Ni-MOF by replacing Ni due to the magnetoelectric coupling effect and Jahn-Teller effect, which results in adjustable polarity of Co x Ni 1-x -MOF. This work provides new insights on how to improve photogenerated charge separation in MOF by enhancing polarization.
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ENERGY & FUELS
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2022
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IF 4.654
Liangkun Hou,Yingying Liu,Kejing Wu,Yingming Zhu,Houfang Lu,Bin Liang
The acid-catalyzed desorption of the MDEA CO2-rich liquid under the electrochemical reaction can lower the desorption temperature, thereby reducing the energy consumption for regeneration. In this work, disodium 4,5-dihydroxy-1,3-benzenedisulfonate (tiron) was used as an acidic medium for the electrocatalytic regeneration of the MDEA CO2-rich solution. The results show that the CO2 desorption efficiency reaches more than 90% at 25 °C for the 0.3 M MDEA (0.1 M tiron) system. At 50 °C, compared with 3 M MDEA (without tiron), the maximum CO2 desorption rate and desorption efficiency of the 3 M MDEA (with 0.1 M tiron) CO2-rich solution increased by 27.4 and 18.3%, respectively. Elevating the temperature can increase the quantity of CO2 desorption and the degree of MDEAH+ deprotonation as well as the reactivity of tiron on the electrode, so the desorption rate of CO2 can be further improved by the oxidation of tiron releasing H+ in coordination with thermal desorption.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
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IF 8.91
Lu Wang,Yaqun Yu,Guoqiang Liu,Junhe Lu
Tetrabromobisphenol S (TBBPS), an emerging brominated flame retardant , can cause neurotoxic and cytotoxic effects to human physiology . In this study, the degradation of TBBPS in Co 2+ activated peroxymonosulfate (PMS) oxidation process was explored. In particular, brominated by-products formed during the degradation of the TBBPS were examined. It was found that TBBPS could be effectively removed in the Co 2+ /PMS oxidation process. The pseudo-first-order rate constants were 0.13 min −1 at 0.2 mM PMS and 0.5 μM Co 2+ initially. It appeared that TBBPS degradation occurred via and HO attacks, but played a dominant role. The presence of natural organic matter (NOM) greatly inhibited the transformation of the TBBPS, which can be explained by the scavenging of the radical species. β-Scission, debromination, and cross-coupling were identified as the main reaction pathways of TBBPS degradation in the Co 2+ /PMS system. Further oxidation and ring-opening of the intermediates generated brominated by-products including bromoform, monobromoacetic acid, and dibromoacetic acid. The formation of the brominated by-products increased gradually in approximately 48 h. But, the presence of NOM reduced the yields of the brominated -by-products. The findings of this study indicate that organic bromine contaminants can be effectively removed but lead to brominated by-products in the activated PMS oxidation process, which should be taken into consideration when -based oxidation technology is applied.
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ChemSusChem
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2022
·Vol. 15
·期 8
·e202200063
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IF 9.14
Qing Ji,Xiaoping Chen,Ya-Jun Cheng,Qingyu Dong,Yanbin Shen,Zhaohui Yang,Binjie Hu,Yonggao Xia
Graphical Carbon, the master : Constructed with unique carbon emcoating structure through CO 2 acivation, NbO 2 benefited from an effective and highly conductive carbon network, giving rise to exceptional electrochemical performances in terms of reversible capacities, rate capability, and cyclic stability. As a promising alternative as lithium-ion anode, niobium dioxide appeals to researchers due to high theoretical capacity and good electron conductivity. However, rarely work about NbO 2 based high performance anode is reported. Here, NbO 2 nanoparticles emcoated in continuous carbon matrix is constructed through CO 2 /H 2 coupling treatment. CO 2 activation introduces unique carbon emcoating structure, which builds interconnected electron conductive network with low carbon content. Furthermore, crystallographic phase of NbO 2 is enhanced during H 2 treatment, which increases the lithium storage ability. Electrochemical performance of NbO 2 anodes is significantly improved based on the carbon emcoating structure. A high reversible capacity of 391 mAh g −1 is retained after 350 cycles at 0.2 C. Additionally, at a current density of 1 A g −1 , the reversible capacity reaches 139 mAh g −1 . Compared with conventional NbO 2 /C nanohybrids, the lithium diffusion coefficient of carbon-emcoated sample shows improvement of three orders of magnitude. Moreover, the in situ XRD investigation shows a reversible lithium insertion behaviour with a limited volume change.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2022
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IF 10.319
Yidu Wang,Jingnan Ding,Jun Zhao,Jiajun Wang,Xiaopeng Han,Yida Deng,Wenbin Hu
Constructing nanohybrids with a synergistic effect using multi-components and specific micro/nanostructures can significantly enhance their electrocatalytic activity. In this work, we fabricated an In 2 O 3 ⊃NC@GO nanohybrid, in which In 2 O 3 nanoparticles (NPs) were encapsulated by an N-doped carbon (NC) shell and supported on graphene. The multi-components in In 2 O 3 ⊃NC@GO synergistically optimize the structural and electronic properties of the material. The particle size and dispersion of In 2 O 3 NPs were optimized owing to the separation effect of the amorphous NC shell and graphene support. This separation effect exposes more number of active sites for the electrochemical reaction. Abundant oxygen vacancies exist in In 2 O 3 , leading to a stronger ability for the adsorption and activation of CO 2 . The NC shell inhibits the direct contact between the electrolyte and In 2 O 3 , which significantly suppresses competitive H 2 evolution. The charge transfer during the electrocatalysis process is also effectively enhanced due to the carbon components. The synergistic effect of multi-components in the In 2 O 3 ⊃NC@GO sample results in a significantly improved CO 2 reduction reaction performance with a high HCOO – Faradic efficiency (FE) of 91.2% and a current density of 40.38 mA cm –2 at –0.8 V obtained using a flow cell. The present work demonstrates that rationally designing nanohybrids with multifunctional components is an effective strategy for optimizing the structural and electrocatalytic properties of materials for energy conversion.
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JOURNAL OF POLYMER RESEARCH
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2022
·Vol. 29
·期 11
·1-12
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IF 3.061
He Zonglin,Xian Wenqi,Ding Zhu,Wang Chaozhi,Huang Zhenhong,Song Lina,Liu Baohua
Propylene carbonate diols (PCD) were synthesized from propylene carbonate and ethylenediamine (EDA), iso-phorone diamine (IPDA) and diethylenetriamine (DETA), respectively. The obtained PCDs were used as extenders to prepare the waterborne polyurethane (WPU). The properties of PCD based WPUs were compared to the that of WPU used butane-1,4-diol (BDO) as extender. The structures of PCDs were characterized by Fourier transform infrared (FTIR) and nuclear magnetic resonance (NMR). The yields, melting points and viscosity of PCDs were tested. The mechanical properties, water absorption, water contact angle, adhesion, pencil hardness, thermal gravimetric analysis (TGA), differential scanning calorimeter (DSC) and dynamic mechanical analysis (DMA) of WPU films were also characterized. The results showed that PCDs with urethane bond in the structure were successfully synthesized and the yields were approximately 99% after 3 h of reaction. Compared to the WPU used BDO as extender, WPU films derived from PCDs exhibited superior tensile strength, outstanding adhesion and pencil hardness, lower water contact angle and water absorption, and higher initial thermal decomposition temperature.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Shangguan Wenchao,Liu Qing,Wang Ying,Sun Ning,Liu Yu,Zhao Rui,Li Yingxuan,Wang Chuanyi,Zhao Jincai
Achieving CO 2 reduction with H 2 O on metal photocatalysts and understanding the corresponding mechanisms at the molecular level are challenging. Herein, we report that quantum-sized Au nanoparticles can photocatalytically reduce CO 2 to CO with the help of H 2 O by electron-hole pairs mainly originating from interband transitions. Notably, the Au photocatalyst shows a CO production rate of 4.73 mmol g −1 h −1 (~100% selectivity), ~2.5 times the rate during CO 2 reduction with H 2 under the same experimental conditions, under low-intensity irradiation at 420 nm. Theoretical and experimental studies reveal that the increased activity is induced by surface Au–O species formed from H 2 O decomposition, which synchronously optimizes the rate-determining steps in the CO 2 reduction and H 2 O oxidation reactions, lowers the energy barriers for the *CO desorption and *OOH formation, and facilitates CO and O 2 production. Our findings provide an in-depth mechanistic understanding for designing active metal photocatalysts for efficient CO 2 reduction with H 2 O.
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Journal of CO2 Utilization
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2022
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IF 8.321
Fei Chen,Wensheng Wei,Yunsheng Gao,Yuxin Wang,Zizhen Yan,Zhanguo Zhang,Haiming Yu,Guangwen Xu,Lei Shi
Ionic liquid 1-ethyl-3-methylimidazolium ([Emim]IM) with high thermal stability and strong basicity was successfully synthesized. Using [Emim]IM as catalyst, dimethyl carbonate (DMC) was directly synthesized from epoxy propane (PO), CO 2 , and methanol under mild reaction conditions. A continuous two-stage DMC synthesis process was developed. The cycloaddition of CO 2 and PO was first conducted to produce propylene carbonate (PC), and then methanol was introduced into the system to synthesize DMC. During the cycloaddition process, 97.40% PO conversion and 97.40% PC yield were achieved with TON of 99.49. In the subsequent transesterification stage, DMC yield attained 83.63% with selectivity higher than 99% and TON of 70.15. [Emim]IM was reused for seven times without obvious deactivation, exhibiting good stability. The effects of reaction temperature, reaction time, the initial pressure of CO 2 , and catalyst weight on cycloaddition and transesterification reactions were systematically investigated. The kinetic study showed that the activation energies (E a ) of cycloaddition and transesterification reactions were 28.02 and 38.53 KJ·mol −1 , respectively, much lower than those of catalysts reported in the literatures. In addition, [Emim]IM displayed superior catalytic activity for the cycloaddition of CO 2 with various epoxy compounds .
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Nano-Micro Letters
·
2022
·Vol. 14
·期 1
·1-13
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IF 23.655
Li Xiaotong,Wang Jianghao,Lv Xiangzhou,Yang Yue,Xu Yifei,Liu Qian,Wu Hao Bin
Dual-site electrocatalysts with in situ formed metal-oxide interfaces are proposed and demonstrated to enhance the formation of multi-carbon products from electrochemical CO 2 reduction.
The 0.5-UiO/Cu delivers a high C2+ Faradaic efficiency of over 74% with notably boosted formation rate and durability, surpassing most reported electrocatalysts.
A unique mechanism of UiO-66 to induce in situ reconstruction of Cu surface and formation of UiO-66-derived amorphous ZrO x /Cu interface is uncovered, which improves the selectivity and productivity toward C2+ products.
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