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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Science Bulletin
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2022
·
IF 20.577
Kunhao Liu,Chao Yang,Ruilin Wei,Xingyu Ma,Chen Peng,Zhengzheng Liu,Yangshen Chen,Yaqin Yan,Miao Kan,Yaoyue Yang,Gengfeng Zheng
Although many catalysts have been reported for the CO 2 electroreduction to C 1 or C 2 chemicals, the insufficient understanding of fundamental correlations among different products still hinders the development of universal catalyst design strategies. Herein, we first discover that the surface *CO coverage is stable over a wide potential range and reveal a linear correlation between the partial current densities of CH 4 and C 2 products in this potential range, also supported by the theoretical kinetic analysis. Based on the mechanism that *CHO is the common intermediate in the formation of both CH 4 (*CHO → CH 4 ) and C 2 (*CHO + *CO → C 2 ), we then unravel that this linear correlation is universal and the slope can be varied by tuning the surface *H or *CO coverage to promote the selectivity of CH 4 or C 2 products, respectively. As proofs-of-concept, using carbon-coated Cu particles, the surface *H coverage can be increased to enhance CH 4 production, presenting a high CO 2 -to-CH 4 Faradaic efficiency ( FE CH 4 ∼52%) and an outstanding CH 4 partial current density of –337 mA cm −2 . On the other hand, using an Ag-doped Cu catalyst, the CO 2 RR selectivity is switched to the C 2 pathway, with a substantially promoted FE C 2 of 79% and a high partial current density of –421 mA cm −2 . Our discovery of tuning intermediate coverages suggests a powerful catalyst design strategy for different CO 2 electroreduction pathways.
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JOURNAL OF MEMBRANE SCIENCE
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2022
·
IF 10.53
Li Yin,Dongfeng Li,Hongxia Guo,Shuai Wang,Tiexin Zhang,Yunling Liu,Fangyuan Gai,Xiaogang Zhao
Incorporating functional materials into polymer precursors is an effective way to prepare carbon molecular sieve (CMS) membranes for solving the trade-off problem between permeability and selectivity of gas separation. In this work, we induced ZIF-8 nanoparticles (from 5 to 20 wt%) as a doping agent to construct a series of phenolphthalein-based cardo poly (arylene ether ketone) (PEK-C) -based hybrid carbon molecular sieve (ZCMS) membranes for CO 2 /N 2 separation via an oxidation and a carbonization process with pyrolysis temperature in the range of 500–700 °C. The carbonized ligand and metal centre of ZIF-8 offered additional pores of carbon matrix, which tailored the ultramicropores of ZCMS membranes for both excellent CO 2 permeability and selectivity. By treating with the temperature of 600 °C, ZCMS-600-15 (ZCMS membrane based on 15 wt% of ZIF-8-doped PEK-C) exhibited the highest CO 2 permeability of 8902 Barrer, which was 1.8 times higher than that of CMS-600 (CMS membrane based on naked PEK-C). ZCMS-600-15 showed an ideal CO 2 /N 2 selectivity value of 42.2, which is also higher than that of other samples, indicating that the appropriate doping amount of ZIF-8 is 15 wt% and the proper carbonization temperature is 600 °C. Moreover, among all the samples, ZCMS-600-15 also showed a superior CO 2 permeability of 8285 Barrer and the highest CO 2 /N 2 selectivity of 24.08 for an equimolar mixture of CO 2 and N 2 , far exceeding the 2008 Robeson upper bound. Therefore, our results suggest that incorporating MOFs into polymer precursors to prepare hybrid carbon molecular sieve membranes by carbonization process could solving the trade-off problem between permeability and selectivity, introducing new possibilities for industrial application.
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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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AICHE JOURNAL
·
2022
·Vol. 68
·期 8
·e17706
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IF 4.167
Qiang Sun,Hongxia Gao,Yu Mao,Teerawat Sema,Sen Liu,Zhiwu Liang
High heat duty is an urgent challenge for industrial applications of amine-based CO 2 capture. The temperature (>110°C) of carbamate breakdown in amine regeneration requires large energy consumption. In this work, we report a novel, stable, efficient, and inexpensive Ni-HZSM-5 catalyst to improve the CO 2 desorption rate and reduce the heat duty. The impregnation method was applied for varying nickel content in the catalysts from 2.16 to 9.80 wt% in HZSM-5. The catalysts were characterized by scanning electron microscope, X-ray powder diffraction, N 2 adsorption–desorption, inductively coupled plasma-optical emission spectrometry, ultraviolet-visible diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, NH 3 -temperature programmed desorption (TPD), Infrared spectroscopy of pyridine adsorption, and Fourier transform infrared spectroscopy. The catalytic performance was evaluated by CO 2 desorption of rich amine solvent at 90°C. It was found that the introduction of nickel increased the acid sites of catalysts compared with parent HZSM-5. This phenomenon plays a key role on improving the CO 2 desorption rate. The density functional theory (DFT) calculations successfully explain the catalytic performance. The catalytic activity associates with the combined properties of MSA × B/L × Ni 2+ . The 7.85-Ni-HZ catalyst presents an excellent catalytic activity for the CO 2 desorption: it increases the amount of desorbed CO 2 up to 36%, reduces the relative heat duty by 27.07% with the same reaction time, and possesses high stability during five cyclic tests. A possible catalytic mechanism for the Ni-HZSM-5 catalysts through assisting carbamate breakdown and promoting CO 2 desorption is proposed based on experimental results and theoretical calculations. Therefore, the results present that the 7.85-Ni-HZ catalyst significantly accelerates the protons transfer in CO 2 desorption and can potentially apply in industrial CO 2 capture.
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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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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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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
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
·
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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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 39
·期 3
·475-483
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IF 3.146
Lv Xia,Li Xueqin,Huang Lu,Ding Siyuan,Lv Yin,Zhang Jinli
Pebax® MH 1657 (Pebax)-based blend membranes with different polyether-amine (PEA) loadings were designed and fabricated for efficient CO 2 separation. The CO 2 separation performance of Pebax/PEA blend membranes was greatly improved in comparison with that of pure membranes. This was mainly because the introduced PEA tailored the physical and chemical microenvironments in blend membranes. Specifically, PEA was a liquid-like additive, which was beneficial to reduce the mass transfer resistance of gases and increase CO 2 permeability. Meanwhile, PEA contained amino groups that acted as mobile carriers to tailor the chemical microenvironment in blend membranes. The mobile carriers preferentially reacted reversibly with CO 2 molecules, facilitating CO 2 transport in membranes. Compared with CO 2 /CH 4 separation performance of pure Pebax membrane, CO 2 permeability and CO 2 /CH 4 separation factor of Pebax/PEA-3 increased by 144.8% and 29.4%, respectively. This study suggests that PEA is a promising membrane material for tailoring the physical and chemical microenvironments in blend membranes for efficient CO 2 separation.
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ChemSusChem
·
2022
·Vol. 15
·期 8
·e202200063
·
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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ChemSusChem
·
2022
·Vol. 15
·期 7
·e202200226
·
IF 9.14
Huaxin Li,Xian Yue,Jing Che,Zhou Xiao,Xianbo Yu,Fenglei Sun,Chao Xue,Junhui Xiang
Graphical Networking at its best : The 3D self-supporting nanonetwork structure of Cu−Bi aerogels provides abundant reactive sites and electron transport channels for efficient electrocatalytic reduction of CO 2 to formate. The electrocatalytic reduction of CO 2 (CO 2 RR) to CO, formate, methane, and other high-value compounds is a promising technique. However, current electrocatalysts suffer from drawbacks such as few active catalytic sites, poor selectivity and low stability, etc, which restrict the practical application. Although monatomic metal catalysts have been widely reported in recent years, high performance non-noble metal aerogels were rarely investigated for electrocatalytic CO 2 RR. Herein, Cu−Bi aerogels with boosted CO 2 RR activity were well constructed by a simple one-step self-assembly method. The resultant Cu 1 Bi 2 exhibits excellent CO 2 RR activity with high faradaic efficiency (FE) of 96.57 % towards HCOOH at a potential of −0.9 V vs. RHE, and the FE HCOOH remains over 80.18 % in a wide potential window (−0.8 V to −1.2 V vs. RHE). It demonstrated that the enhanced CO 2 RR activity of Cu−Bi aerogels could be attributed to the 3D self-supporting structure of the catalysis, synergistic effect, and low interfacial charge transfer resistance.
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