APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Nanhui Li,Ping Yan,Yuanhao Tang,Jianghao Wang,Xin-Yao Yu,Hao Bin Wu
Electrochemical reduction of carbon dioxide provides a feasible solution to the energy and climate crisis. Bi-based catalysts are promising candidates to electrochemically convert carbon dioxide (CO 2 ) into formic acid or formate. Herein, ligand-stabilized Bi nanosheets are obtained from in-situ electrochemical reduction of a Bi-based metal-organic framework, which exhibit remarkable electrocatalytic performance for CO 2 reduction. A high Faradic efficiency of 98 % for formate is achieved at a potential of -0.80 V vs . reversible hydrogen electrode (RHE) with an improved durability over 40 h. The remarkable electrocatalytic activity and stability could be attributed to the in-situ generated catalyst with abundant under-coordinated Bi active sites, which are effectively stabilized by residual ligands adsorbed on surface. This study demonstrates that ligand-stabilized under-coordinated surface sites would be facilely generated from in-situ transformation of metal-organic precursors for highly efficient CO 2 conversion.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yan Zhang,Haryo Wibowo,Li Zhong,Mika Horttanainen,Zunbo Wang,Caimeng Yu,Mi Yan
High CO 2 content exists in the raw syngas produced from supercritical water gasification of food waste, CO 2 removal to improve quality of the syngas is necessary before further utilization. In this study, Cu-BTC, Mg/Cu-BTC, Cu-BTC@MWCNT, and Mg/Cu-BTC@MWCNT were synthesized and characterized as CO 2 adsorbents. The adsorption experiments were conducted to investigate the optimal adsorbent and adsorption conditions. The results indicated that Mg 2+ and multi-walled carbon nanotubes (MWCNT) doped into Cu-BTC influenced the physical properties of adsorbents. Among of all studied adsorbents, Mg/Cu-BTC@MWCNT had the maximum CO 2 adsorption capacity (3.63 mmol/g) and selectivity (14.28) at 25 °C and 100 kPa. Analysis of variance (ANOVA) exhibited that adsorption pressure had significant effects on CO 2 adsorption capacity of Mg/Cu-BTC@MWCNT. The influences of different operating parameters on CO 2 adsorption capacity and selectivity were discussed in Mg/Cu-BTC@MWCNT. The adsorption isotherms of gas components on Mg/Cu-BTC@MWCNT can be sorted as follows: CO 2 > CO > CH 4 > H 2 . In additional, the regeneration experiment with 5 times was conducted and the result showed that Mg/Cu-BTC@MWCNT has high stability.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Xinyue Ma,Jianjun Du,Hao Sun,Fenghui Ye,Xin Wang,Pengfei Xu,Chuangang Hu,Lipeng Zhang,Dong Liu
Efficient and cost-effective electrocatalysts for CO 2 reduction with high selectivity are desirable but remain challenging. Herein, a low-cost and efficient electrocatalyst composed of boron, nitrogen co-doped mesoporous carbon (BNMC) for CO 2 reduction reaction (CO 2 RR) along with the catalytic mechanism are reported. The resultant BNMC (i.e., BNMC-1000) exhibits good CO 2 RR activity with high Faradaic efficiency (FE, 95%) towards CO at low overpotential (423 mV). It is demonstrated that the codoping of nitrogen and boron atom, and the mesopore structure are favorable to the excellent catalytic activity of CO 2 RR. The doped boron atom cooperate with nitrogen atom could adjust the projected density of states of the carbon active site generating a proper adsorbed energy of *COOH and *CO on the carbon surface. This work offers a basic guide for developing metal-free carbon-based CO 2 RR electrocatalysts with high-performance.
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高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2021
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IF 6.064
Ying Yang,Kai Chen,Liang Huang,Min Li,Taiping Zhang,Mi Zhong,Ping Ning,Junya Wang,Shikun Wen
It has been reported that the addition of graphene oxide (GO) can increase the dispersion and heterogeneous nucleation of layered double hydroxide (LDH), thus providing more active sites, which is more conducive to CO 2 adsorption. Herein, we reported alkali metal nitrates ((Li 0.3 Na 0.18 K 0.52 )NO 3 ) promoted LDH and GO composites (LDH/GO) as adsorbents for CO 2 capture. The influence of mass ratio of LDH to GO, the impregnation ratio of alkali metal nitrates, the calcination and adsorption temperature, as well as the cycling stability were investigated systematically. The results indicated that the CO 2 capture capacity of LDH/GO composite with 30 mol% (Li 0.3 Na 0.18 K 0.52 )NO 3 could reach 4.51 mmol·g −1 , which was 5.86 times higher than LDH/GO1 without loading alkali metal nitrates. Moreover, it had outstanding CO 2 adsorption capacity in the range from 200 °C to 320 °C. In addition, the cyclic adsorption and desorption test manifested that the CO 2 uptake of the material can reach 3.07 mmol·g −1 after 22 cycles. We believe that this study will give a significant contribution to fabrication of LDH based composites as CO 2 adsorbents in future study.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xiaoyi Gao,Xin Li,Siyi Cheng,Bihong Lv,Guohua Jing,Zuoming Zhou
The main issues in the application of biphasic amine absorbent include the inconvenient separation of the liquid–liquid biphase and the clogging that is associated with the solid–liquid mixture. A novel solid–liquid ‘phase controllable’ biphasic amine absorbent was therefore developed, in which the phase separation occurred only when the absorbent was near saturation. The absorbent, composed of triethylene tetramine (TETA), 2-amino-2-methyl-1-propanol (AMP), and N-methylformamide (NMF), turned into solid–liquid biphase under CO 2 loading of 0.85 mol mol −1 , which is close to saturation (0.92 mol mol −1 ). The solid phase comprised white powder that accounted for only 42 % of the total volume while absorbing 91 % of the total load. Turbidity and particle size tests showed that the phase separation was self-aggregating. The mechanisms of absorption and regulation were obtained using 13 C NMR and molecular simulation. During the absorption, CO 2 first combined with TETA to generate TETAH + CO 2 – /TETACO 2 – through the zwitterion mechanism, and then combined with AMP to generate AMPCO 2 – because of the lower reaction activity between CO 2 and AMP. The TETA-carbamate was found to greatly weakened the strength of the hydrogen bonds and the van der Waals forces between AMPH + and AMPCO 2 – , increasing the solubility of the intermediate products, and therefore achieved the purpose of controlling the phases separation inherent in the reaction.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
HaiyanYang,Xinzhong Wang,Jun Liu,Wanzhen Liu,Yue Gong,Yankun Sun
Solid amine materials are promising adsorbents for CO 2 capture from biogas , flue gas and other similar gas mixture. Here, tetraethylenepentamine (TEPA)-impregnated porous polymeric resin (ADS-17) with very high CO 2 adsorption capacity was successfully prepared. Its CO 2 separation performance from simulated biogas was investigated by breakthrough experiments. And the influence of parameters such as TEPA loading, adsorption temperature and flow rate on the adsorption behaviours were studied in detail. The optimal TEPA loading was 40 wt% (ADS-17–40%TEPA) and the CO 2 adsorption capacity of this adsorbent reached the optimal value (ca. 264.2 mg▪g −1 ) at the flow rate of 200 mL▪min −1 . The CO 2 adsorption capacity of ADS-17–40%TEPA had no pronounced change from 25 °C to 70 °C, but it decreased obviously when the adsorbent was heated to 90 °C. At 100 °C, the adsorption capacity became negligible. According to detailed characterization, it was inferred that the pores of ADS-17–40%TEPA in the range of 13–115 nm were probably responsible for CO 2 diffusion. In addition, ADS-17–40%TEPA possessed good reversibility and the CO 2 adsorption capacity was nearly stable after two adsorption–desorption cycles. ADS-17–40%TEPA with high and fast CO 2 adsorption exhibits a very promising application in CO 2 separation from biogas.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Lizhi Wang,Jiangfei Guo,Xiyuan Xiang,Yafei Sang,Jianhan Huang
Functionalized porous organic polymers (POPs) with high Brunauer-Emmett-Teller (BET) surface area ( S BET ) and unique porosity is promising while its facile synthesis remains a challenge. Herein, a novel synthesis strategy based on Schiff-base chemistry was developed and melamine was embedded as a rigid external cross-linker to construct a kind of novel functionalized POPs. The resulting melamine-supported polymers showed high S BET (645 m 2 /g) and total pore volume ( V total , 0.84 cm 3 /g) with unique hierarchical porosity, indicative of its outstanding CO 2 capture and Hg 2+ removal. Noticeably, the as-prepared sample TPE-TMC-2MA exhibited high CO 2 uptake of 153 mg/g and its ultramicropore volume ( V ultra , 0.16 cm 3 /g) played a positive role. In particular, the maximum capacity of Hg 2+ reached 392 mg/g, much higher than some other materials reported in the literature.
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ACS Sustainable Chemistry & Engineering
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2019
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IF 6.97
Wenrui Wan,Dazhen Xiong,Qian Zhang,Jianji Wang
It is very important to develop “smart” solvents that can integrate the advantages of homogeneous and heterogeneous reactions into one chemical process for enhanced reaction rate and minimal environmental impact. In designing these solvents, the applicability of the systems to real processes strongly depends on the phase behavior of the systems. In this work, a novel class of CO2-driven miscible–immiscible transition of deep eutectic solvents (DESs) has been explored. These DESs are composed of alkanolamine compounds as hydrogen-bond acceptors (HBAs) and phenolic compounds as hydrogen-bond donors (HBDs). They exhibit unique phase behavior with H2O: miscible with water in the absence of CO2 but immiscible with water in the presence of CO2 at room temperature and ambient pressure. Reversible liquid–liquid phase transition of such DES–H2O mixtures can be realized by alternative bubbling of CO2 and N2 under ambient conditions. Spectroscopic investigations show that the mechanism behind the miscible–immiscible transition of DESs involves breaking of the hydrogen bonds between HBDs and HBAs by H2CO3 generated by bubbling CO2 through an aqueous solution because the acidity of H2CO3 is stronger than that of HBAs. Further, the HBAs react with H2CO3 to form ammonium salts. The salting-out effect of ammonium salts leads to the formation of an ammonium salt-rich top phase and an HBD-rich bottom phase. When CO2 is removed by bubbling of N2, a reversible process is achieved.
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CHEMICAL ENGINEERING SCIENCE
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2019
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IF 3.372
Zihan Qu,Hong Wu,Yue Zhou,Leixin Yang,Xingyu Wu,Yingzhen Wu,Yanxiong Ren,Ning Zhang,Yutao Liu,Zhongyi Jiang
Membranes with fast CO 2 transport pathways have attracted intense attention due to their outstanding CO 2 permeability, showing potential for industrial application. Regulating the spatial distribution of CO 2 -philic groups in polymer-based membranes is expected to be a promising strategy to achieve the fast CO 2 transport pathways. In membrane matrix, the interconnected network of concentrated domains of CO 2 facilitated transport groups provides membranes with specific CO 2 transport pathways and finally leads to their high separation performance. In this study, a novel kind of polyelectrolyte membrane, quaternary ammonium polysulfone with interconnected ionic clusters, is prepared to enhance the CO 2 permeability. The hydrophilic quaternary ammonium groups tend to aggregate spontaneously to create ionic clusters. Furthermore, under humidified conditions, these ionic clusters are connected by water to form an ionic cluster network in the membrane matrix. The ionic cluster network plays the crucial role in accelerating the selective transport for CO 2 molecules over CH 4 by the reversible interaction between CO 2 and ion pairs. By tuning the quaternization degree of polysulfone, a series of polyelectrolyte membranes with different size of ionic clusters were developed. Membranes with hydrated ionic clusters (5–9 nm) show dramatic enhancement in CO 2 separation performance, especially in CO 2 permeability. The as-prepared quaternary ammonium polysulfone membrane with 8.98 nm ionic clusters exhibited the high CO 2 permeability of 1109.44 Barrer and a high CO 2 /CH 4 selectivity of 29.70, which exceeds 2008 Robeson upper bound limit. The optimized separation performance of QA-PSf membranes is attractive for potential application such as CO 2 capture from flue gas and natural gas.
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ACS Applied Materials & Interfaces
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2019
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IF 8.456
Shiyu Bie,Meili Du,Wenxiang He,Huigang Zhang,Zhentao Yu,Jianguo Liu,Meng Liu,Wuwei Yan,Liang Zhou,Zhigang Zou
Efficient electrocatalysts for Li2CO3 decomposition play an important role in Li–CO2 batteries. In this paper, carbon nanotubes (CNTs) decorated with RuO2 is firstly introduced as cathode materials for Li–CO2 batteries. The CNT@RuO2 composite can not only deliver a high specific capacity but also a lower charge voltage. With the CNT@RuO2 cathodes, the Coulombic efficiency still remains around 100% until the 15th cycle. The charge voltage of early 30 cycles at a current of 50 mA·g–1 with a capacity limit of 500 mAh·g–1 can be fully lowered under 4.0 V. Particularly, the CNT@RuO2 cathode can realize most decomposition of prefilled Li2CO3 and show a platform at around 3.9 V. This catalytic activity toward both in situ formed and preloaded Li2CO3 is more feasible for practical application in complex environment.
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PubMed
高影响因子
Small
·
2019
·Vol. 15
·期 17
·1900289
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IF 10.856
Hao Dong,Lei Zhang,Lulu Li,Wanyu Deng,Congling Hu,Zhi-Jian Zhao,Jinlong Gong
The electroreduction of CO 2 to CO provides a potential way to solve the environmental problems caused by excess fossil fuel utilization. Loading transition metals on metal oxides is an efficient strategy for CO 2 electroreduction as well as for reducing metal usage. However, it needs a great potential to overcome the energy barrier to increase CO selectivity. This paper describes how 8.7 wt% gold nanoparticles (NPs) loaded on CeO x nanosheets (NSs) with high Ce 3+ concentration effectively decrease the overpotential for CO 2 electroreduction. The 3.6 nm gold NPs on CeO x NSs containing 47.3% Ce 3+ achieve CO faradaic efficiency of 90.1% at −0.5 V in 0.1 m KHCO 3 solution. Furthermore, the CO 2 electroreduction activity shows a strong relationship with the fractions of Ce 3+ on Au-CeO x NSs, which has never been reported. In situ surface-enhanced infrared absorption spectroscopy shows that Au-CeO x NSs with high Ce 3+ concentration promote CO 2 activation and *COOH formation. Theoretical calculations also indicate that the improved performance is attributed to the enhanced *COOH formation on Au-CeO x NSs with high Ce 3+ fraction.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2019
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IF 3.131
Zihao Yang,Wei Wu,Zhaoxia Dong,Meiqin Lin,Shuwei Zhang,Juan Zhang
The establishment of a miscible phase between CO 2 and crude oil can significantly improve CO 2 flooding efficiency. However, the minimum miscibility pressure (MMP) between CO 2 and crude oil is usually higher than the fracture pressure of the formation, how to reduce the MMP between CO 2 and crude oil is very important, and there are fewer related studies. Our inspiration for reducing MMP comes from the unique dispersion characteristics of CO 2 in alcohol, the intermolecular force of crude oil may decrease due to the existence of alcohols. In this paper, the CO 2 solubility and the oil volume expansion with adding a variety of alcohols (1-butanol, 1-pentanol and 1-hexanol) were measured by a visible high temperature and high pressure cell from 7 MPa to 20 MPa at 343.15 K. The MMP between CO 2 and crude oil is predicted by measuring the interfacial tension (IFT) between CO 2 and crude oil from 2 MPa to 43.3 MPa at 343.15 K. The results showed that the CO 2 solubility in crude oil and the oil volume expansion were greatly improved due to the addition of alcohols. Especially 1-butanol, 1-pentanol and 1-hexanol were mixed by 8:1:1(volume ratio), 5% (volume ratio) alcohols mixture was added to the crude oil, the CO 2 solubility in crude oil increased by 28.74% at 345.15 K and 19 MPa, and the volume expansion coefficient of crude oil also increased by 4.45% at 345.15 K and 14 MPa. It is encouraging to note that the MMP between CO 2 and crude oil decreases by 9.21% after adding 5% alcohols mixture into crude oil. This article is able to provide a new technique for reducing the MMP between CO 2 and crude oil in the field of enhanced oil recovery.
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