APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Juan Yang,Yanpeng Dou,Huimeng Yang,Dihua Wang
High-performance adsorbents derived from wastes are of paramount significance for environmental remediation and value-added utilization. Herein, a novel porous carbon (i.e. electrolytic carbon, EC), prepared from greenhouse gas (CO 2 ) by electrochemical reduction in molten carbonate, was investigated as an efficient adsorbent to remove tetracycline (TC) from water. The EC possessed oxygen-containing functional groups, large specific surface area (1064.8 m 2 g −1 ), high pore volume (1.87 cm 3 g −1 ), and rich mesopore, availing the removal of bulky TC. A rapid adsorption equilibrium (within 1 h) and a high removal efficiency (98.7%) were obtained. Moreover, the adsorption was an exothermic reaction and the whole process obeyed the pseudo-second-order kinetic and Langmuir models, gaining a saturated adsorption capacity of 393.5 mg g −1 at 25 °C, which was superior to various reported biochar and commercial carbon materials. Besides, the adsorption of EC exhibited a wide pH adaptability ranged from 2 to 9, and excellent recyclability. A π-π interaction was identified as the predominant mechanism by investigating the adsorption performance of EC and IR, XPS characterizations. These results highlight significant implication for the future application of CO 2 -derived carbon adsorbents in the treatment of antibiotic wastewater.
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高影响因子
FUEL
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2020
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IF 5.578
Long Ma,Shuzhen Chen,Changlei Qin,Susu Chen,Weiyang Yuan,Xu Zhou,Jingyu Ran
Li 4 SiO 4 is a well-acknowledged CO 2 sorbent in the sorption-enhanced reforming system for low-cost H 2 production with a high purity. However, the inevitable presence of H 2 S in the biomass-derived syngas etc. could possibly affect the in-situ CO 2 adsorption significantly, which is important but has never been reported. In this work, the adsorption of CO 2 using Li 4 SiO 4 was investigated under varying H 2 S concentrations and reaction temperatures, and a series of characterization techniques were utilized to understand the effect of H 2 S and its action mechanism. The results show that the presence of H 2 S causes a rapid loss-in-capacity of Li 4 SiO 4 in capturing CO 2 during the cyclic reactions, and a higher concentration greatly exacerbates the problem. Moreover, the negative impact of H 2 S is found to have a strong relationship to the reaction temperature. It is proposed that at 325~475 °C, Li 4 SiO 4 and H 2 S react to form bits of Li 2 S and some kinds of sulfates, and at 625~775 °C, a large amount of dense KLiSO 4 is generated covering the surface of the sorbent. In contrast, at a high temperature above 925 °C, sintering of Li 4 SiO 4 plays a critical role, leading to a significant change on its microstructure.
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高影响因子
ENERGY
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2020
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IF 6.082
Fa-Ping Liu,Ai-Rong Li,Jie Wang,Ze-Dong Luo
Hydrate technology is a promising alternative method for carbon dioxide (CO 2 ) capture and storage from flue gas . In order to promote the hydrate growth rate and increase gas storage capacity, CO 2 hydrate nucleation and growth induced by iron-based ionic liquid ([BMIM][FeCl 4 ]) was studied with 400 rpm rotation speed at a temperature of 274.15 K and initial pressure of 5.0 MPa in this work. The induction time of CO 2 hydrate formation was decreased by 52.8% and the storage capacity of CO 2 hydrate was increased by 13.7% in 25.0 g/L [BMIM][FeCl 4 ] solution. The local hydrogen bonds are strengthened by the combination interaction between the complex anion ([FeCl 4 ] − ) and water (H 2 O) molecules, which is favorable to the ordered arrangement and the proton exchange rate of H 2 O molecules during the hydrate nucleation. Besides, large mass transfer channels are formed by the large molar volume and regular tetrahedral structure of [FeCl 4 ] − during the hydrate growth, which improves the diffusion rate of CO 2 and H 2 O molecules in the solution to promote the hydrate growth. Distribution of lipophilic cation and hydrophilic anion with a large molecular volume of [BMIM][FeCl 4 ] at the gas-liquid interface hinders the formation of cage structure of H 2 O molecules.
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高影响因子
Nature Communications
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2020
·Vol. 11
·期 1
·1-8
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IF 12.121
Feng Jiaqi,Gao Hongshuai,Zheng Lirong,Chen Zhipeng,Zeng Shaojuan,Jiang Chongyang,Dong Haifeng,Liu Licheng,Zhang Suojiang,Zhang Xiangping
Developing effective catalysts based on earth abundant elements is critical for CO 2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO ( j CO ) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N 3 site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a j CO of 14.0 mA cm −2 at a low overpotential of 0.44 V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher j CO of 29.7 mA cm −2 is obtained in an ionic liquid electrolyte at 0.62 V overpotential. In situ X-ray absorption spectra and density functional theory calculations demonstrate that the remarkable performance of the catalyst is attributed to the Mn-N 3 site, which facilitates the formation of the key intermediate COOH * through a lowered free energy barrier.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Shikang Yin,Linlin Sun,Yaju Zhou,Xin Li,Jinze Li,Xianghai Song,Pengwei Huo,Huiqin Wang,Yongsheng Yan
The use of semiconductor photocatalytic reduction technology has higher efficiency and lower energy consumption for CO 2 reduction, but its existence of some mismatched energy band positions and relatively slow charge-hole separation greatly limits its practical application. In this paper, a SnS 2 /Au/g-C 3 N 4 embedded structure model with carbon and nitrogen hybridization is proposed to gain an in-depth understanding of the role of hybridization and precious metal modification in photocatalysis. Carriers were investigated from the perspective of kinetics through photocurrent, LSV curve, and FL spectroscopy. After modification of Au nanoparticles, the photo-excited electrons showed a slower decay process, indicating that the separation of carriers was enhanced, which was further confirmed by impedance and PL spectroscopy. SEM, AFM and TEM analysis confirmed that the 2D face-to-face SnS 2 /Au/g-C 3 N 4 embedded structure was successfully prepared and the Au nanoparticles were evenly distributed. Au nanoparticles not only act as a bridge for electron transport in 2D semiconductor materials to accelerate electron transport, but generate more excited electrons by themselves under the radiation of sunlight, which effectively improves the separation efficiency of electron-hole pairs and enhances the photocatalyst activity. DFT calculations show that the Z-type mechanism and the intercalated energy level of the SnS 2 /Au/g-C 3 N 4 embedded structure expand the light absorption and improve the carrier separation efficiency. As expected, the photocatalyst activity with CO and CH 4 the evolution rate of up 93.81 µmol·g −1 ·h −1 and 74.98 µmol·g −1 ·h −1 under visible light irradiation, respectively, while the photocatalytic activity is negligible loss after 30 h photoreduction. This work reveals the role of embedded structure and precious metal modification in the separation and transmission of electron-hole, opening up new perspective for achieving high-efficiency solar CO 2 reduction performance.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Xueru Wang,Juzheng Song,Yan Chen,Hang Xiao,Xiaoyang Shi,Yilun Liu,Liangliang Zhu,Ya-Ling He,Xi Chen
The moisture-swing sorbent of amine-based anion exchange resins is one of the most promising materials for direct carbon capture from ambient air to alleviate excessive emissions of CO2. In this study, how the physical and chemical properties of amine-based anion exchange resins affect their carbon capture performances is studied systematically, through different kinds of resins. Contrary to previous understandings, the effect of the chemical functional groups on the overall capture performance is found to far outweigh that of the physical properties. It is found that the main property that determines the absorption capacity is the chemical one, i.e., the amine functional groups, while properties dominating the absorption kinetics are the physical ones, i.e., particle size and microporous structures. The absorption capacity of resins loaded with strong amine groups is strikingly higher than that with weak amine groups. The mechanism is explored by a combination of molecular dynamics and quantum chemical calculations. The most superior sorbent is the macro-porous strong base resin due to its strong amine groups and large inner pore sizes. The present study provides new insights into selecting suitable absorbents or preparing better ones for enhanced direct air capture of CO2.
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高影响因子
Materials Advances
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2020
·Vol. 2
·期 2
·692-699
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IF 0
Fangyuan Gai,Dongying Zhu,Yunhuan Wu,Xiaogang Zhao,Changhai Liang,Zhenguo Liu,Yunling Liu,Tonghua Wang
Striking a balance between the nitrogen content and pore texture of N-containing metal–organic framework (MOF)-derived carbon is a considerable challenge for high-performance CO2 capture. The high-temperature pyrolysis and activation facilitated well-developed pore structures but resulted in serious nitrogen loss of MOFs. In this work, we developed MOF (ZIF-8)-derived N-doped porous carbons (NPCs) by integrating ZIF-8 with pomelo peel via a co-carbonization and activation process to construct a high-performance CO2 adsorbent. The pomelo peel can effectively prevent the nitrogen loss from the ZIF-8 backbone via pre-melting and polymerization and simultaneously offer the ideal porosity and BET surface area during the co-carbonization and activation process. By tuning the ZIF-8 loading capacity and the activation temperature, the sample NPC-800-4 prepared at 800 °C possessed both ultrahigh surface area (∼1967 m2 g−1) and high N content (∼13.15 wt%). Particularly, the CO2 capacity of NPC-800-4 reached 5.51 mmol g−1 at 25 °C and 9.01 mmol g−1 at 0 °C under 1 bar due to its relatively high content of pyrrolic-N (N5 ∼ 61.2%) and pyridinic-N (N6 ∼ 16.5%), as well as the proper pore size distribution (0.64 nm). In addition, the TPD measurement and CO2 adsorption energy (Qst) of NPC-800-4 also suggested the high desorption activation temperature and energy, indicating a strong binding capacity toward CO2. Moreover, NPC-800-4 exhibited almost constant CO2 uptake in 8 consecutive adsorption–desorption cycles, indicating that the sample with great stability and recyclability would be easily adapted and recycled from industries. This co-carbonization and activation strategy to assembly MOFs with biomass would pave the way for enhancing CO2 capture of MOF-derived carbons.
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Journal of CO2 Utilization
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2021
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IF 7.132
Tianhao Wang,Yi Zhao,Huiru Zhang,Weitian Hui
Carbon dioxide (CO 2 ) emissions from the combustion of fossil fuels cause the intensification of greenhouse effect. Consequently, a new non-noble nanoalloy of Ni 0 , Cu 0 and Fe 0 was prepared for the production of formate (HCO 2 − ) from CO 2 in flue gas by hydride transfer reaction under atmospheric pressure and mild temperature in this work. Under the optimal reaction conditions obtained by experimental optimization, which were that catalyst dosage was 1 g·L -1 , KBH 4 concentration was 0.15 mol·L -1 , reaction temperature was 55 °C, solution pH was 9.5 and flow velocity of flue gas was 0.5 L min -1 , the CO 2 conversion efficiency (CCE) was achieved as 55.97 %. Due to the employment of nanoalloy of Ni 0 , Cu 0 and Fe 0 , the CCE was improved by about 25 % compared with that in non-catalytic conditions, and meanwhile, the KBH 4 dosage was reduced by around 45 %. Based on the catalyst properties before and after the reaction as well as the product detection, we put forward that the electrode potential differences among the ternary transition metals resulted in the improvement of catalyst surface activity to promote KBH 4 activation and the hydride transfer reaction for CO 2 . The work presented herein is conducive to the development of novel transition metal-based nanomaterials for CO 2 resource utilization in a low-energy way.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Qingqing Hou,Xiyi Li,Yunhong Pi,Jing Xiao
Photocatalytic conversion of CO2 into fuel and value-added chemicals as a promising method has been applied recently to ease energy- or environment-related crises. Herein, we construct an In2S3@NH2-MIL-68(In)@In2S3 (denoted as SMS(In)) sandwich homologous heterojunction via a controllable in situ metal–organic frameworks (MOF) sulfuration process. The improved photoreduction activity mainly lies in the effective charge transfer and separation through a homogeneous interface, enhanced CO2 adsorption and mass transfer, and plentiful reactive sites. Benefiting from this unique hollow homologous heterojunction, SMS(In)-7 obtains a CO generation rate as high as 11.23 μmol g–1 h–1 with visible-light irradiation, nearly 3 times enhancement over that of pure MOF-derived In2S3. This work provides a novel insight into the utilization of MOF-based platform for an efficient atomically heterojunction design.
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高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2020
·Vol. 45
·期 4
·6273-6284
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IF 3.741
Xiaolin Shao,Qi Zhang,Xurui Zhang,Jin Yi,Yuyu Liu,Jiujun Zhang
Summary A facile method is developed to fabricate nanoporous, structured, Sn-based catalyst electrodes. Sn, Zn, and multiwalled carbon nanotubes (MWCNTs) are co-electrodeposited on a copper substrate, followed by chemical dezincification in NaOH aqueous solution to remove Zn. By controlling variables such as the contents of Zn and MWCNTs, a series of Sn-MWCNT/Cu (S Z MC) electrodes are fabricated. Experimental results show that using such novel S Z MC electrodes can achieve a HCOO − Faradaic efficiency of over 91% at −0.99 V versus RHE for 10 hours in CO 2 -saturated 0.5 M KHCO 3 aqueous solution. The high performance is attributed to the addition of MWCNTs and Zn, followed by chemical dezincification to remove Zn and then create vacancies in the catalyst structure, which results in a special porous structure of S Z MC with large surface area. Then ECSA is used for enhancing the catalytic activity and selectivity of HCOO − production, as well as promoting intermediate adsorption and mass transfer.
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高影响因子
Journal of Energy Chemistry
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2020
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IF 7.216
Shuangxi Lin,Ziwen Hao,Jindong Shen,Xiao Chang,Shouying Huang,Maoshuai Li,Xinbin Ma
The metal-support interaction is of critical importance to enhance the catalytic activity and selectivity. However, it is still challenging to construct an appropriate interaction starting from the catalyst fabrication and/or activation. We herein established low-temperature treatment of Ni 2+ ions impregnated on ceria in reductive atmosphere and reduction–oxidation cycles as effective approachs to regulate the metal-support interaction and raise the catalytic performance in the CO 2 methanation. The proposed construction approach yielded Ni/CeO 2 that displayed highly dispersed Ni nanoparticles in contact with CeO 2 (111) and (100) facet, higher density of surface oxygen vacancies and larger amounts of weak basic sites relative to the reference samples, which increased the capacity for H 2 and CO 2 adsorption/activation. The interaction resulted in appreciably (2–3 fold) higher activity in the CO 2 methanation with maintaining almost full selectivity to CH 4 and high stability. Coverage of Ni surface by CeO 2− x thin layer as a typical structure of strong metal-support interaction resulting from high-temperature reduction, can be alleviated via reduction–oxidation cycles. We also demonstrate the activation treatment-determined metal-support interaction effect can generally extend to (TiO 2 and ZrO 2 ) supported Ni catalysts.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Guohui Li,Yuanyuan Sun,Qingming Zhang,Zhe Gao,Wei Sun,Xiaoxia Zhou
Photocatalytic reduction of CO 2 into high added-value chemical products has received special attention. Herein, we designed a novel hierarchically porous and defective TiO 2 modified by Ag quantum dots via a hydrothermal process assisted with organic surfactant and subsequently in-situ photodeposition method. The obtained Ag quantum dots modified TiO 2 (Ag/TiO 2 ) shows excellent and stable photocatalytic activity in CO 2 reduction. In addition, the competing H 2 evolution can be completely suppressed. The super photocatalytic activity can be ascribed to the design of hierarchically porous, the intrinsic defects in TiO 2 , the localized surface plasmon resonance of Ag and the synergetic effect between Ag quantum dots and defective TiO 2 , which jointly improves the CO 2 adsorption performance, enhances visible light absorption capacity and accelerates the separation of photogenerated charges. This work may provide a strategy to design and synthesis defective and hierarchically porous metal oxides for photocatalytic CO 2 reduction.
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