APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Yifan Li,Chang Chen,Rui Cao,Ziwei Pan,Hua He,Kebin Zhou
Electrochemical reduction of CO 2 into value-added carbon compounds offers a promising strategy to mitigate global warming, but present challenges for chemistry due to the poor selectivity and stability of electrocatalysts. In this work, we report a dual-atom Ag 2 /graphene catalyst featuring well-defined AgN 3 -AgN 3 active site for CO 2 electrochemical reduction. This dual-atom catalyst can drive CO 2 reduction reaction at a potential as high as -0.25 V, and exhibit excellent CO Faradic efficiency up to 93.4 % with a current density of 11.87 mA cm −2 at -0.7 V and long-term stability, far surpassing the single-atom Ag 1 /graphene and the traditional silver nanoparticle catalysts. DFT calculations reveal that the dual-atom Ag site lowers the barrier for the formation of *COOH by stabilizing the *CO 2 through the concomitant interactions with the C and an O atom of CO 2 , resulting in excellent catalytic performance.
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AICHE JOURNAL
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2020
·Vol. 66
·期 11
·e16645
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IF 3.519
Meng-Meng Jin,Yu-Xia Li,Chen Gu,Xiao-Qin Liu,Lin-Bing Sun
Due to the excellent adsorption capacity on CO 2 , Mg-MOF-74 is highly potential for carbon capture. However, the practical application is seriously hindered by the poor hydrolytic stability of Mg-MOF-74 even towards trace of moisture. Here we report a strategy by adjusting the microenvironment of Mg-MOF-74 from hydrophilic to superhydrophobic by coating polydimethylsiloxane (PDS, yielding M74@P), which markedly enhances the hydrolytic stability. Mg-MOF-74 is degraded obviously upon exposure to humid atmosphere (75% relative humidity) for 7 days, while M74@P retains its structure well even after 1 year. The dynamic breakthrough results show that the optimized M74@P sample can capture 6.65 mmol g −1 CO 2 from wet CO 2 /N 2 mixtures after 100 cycles, which is superior to Mg-MOF-74 (1.17 mmol g − 1 ) and most reported adsorbents under comparable conditions (continuous flow adsorption from wet gases). The excellent adsorption capacity and hydrolytic stability make the present adsorbents highly promising for practical applications in carbon capture.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Yanxia Zhu,Jun Cheng,Xiaodan Xu,Hongxiang Lu,Yangang Wang,Xi Li,Weijuan Yang
CO 2 capture with microalgae has been put forward in response to global concern on greenhouse gas emission . However, the short residence time and slow diffusion of CO 2 in water limits the growth of microalgae. In order to improve CO 2 transfer from gas phase to liquid phase and utilization by algal cells, polyethylene glycol 200 (PEG 200) was used as CO 2 absorbent to promote growth of Nannochloropsis oceanica with the bubbling of 15 vol% CO 2 . Total inorganic carbon (TIC) absorbed in culture medium remained constant at 5.6 mM when 15 vol% CO 2 was bubbled continuously. PEG 200 in the medium provided additional CO 2 absorption from 0.6 to 4.8 mM when PEG 200 concentration increased from 0.5 to 4 mM. The specific growth rate of N. oceanica reached the maximum (1.41 d −1 ) with 1 mM PEG 200 in culture medium, which was 21.5% higher than the specific growth rate without PEG 200. About 79% of the increase in biomass was attributed to the increased TIC with more CO 2 dissolution in culture medium because of PEG 200, and about 21% was attributed to PEG 200 itself utilized as an organic carbon source. In conclusion, PEG 200 as a CO 2 absorbent can effectively capture flue-gas CO 2 for algal growth.
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CHEMISTRY OF MATERIALS
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2020
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IF 9.567
Zhoujie Chen,Yangguang Hu,Jin Wang,Qing Shen,Yaohong Zhang,Chao Ding,Yu Bai,Guocan Jiang,Zhengquan Li,Nikolai Gaponik
Converting CO2 into chemical fuels with a photocatalyst and sunlight is an appealing approach to address climate deterioration and energy crisis. Metal complexes are superb candidates for CO2 reduction due to their tunable catalytic sites with high activity. The coupling of metal complexes with organic photosensitizers is regarded as a common strategy for establishing photocatalytic systems for visible-light-driven CO2 reduction. While most of the organic photosensitizers generally contain precious metals and are available through onerous synthetic routes, their large-scale application in the photocatalysis is limited. Halide perovskite nanocrystals (NCs) have been considered as one of the most promising light-harvesting materials to replace the organic photosensitizers due to their tunable light absorption range, low cost, abundant surface sites, and high molar extinction coefficient. Herein, we demonstrate a facile strategy to immobilize [Ni(terpy)2]2+ (Ni(tpy)) on inorganic ligand-capped CsPbBr3 NCs and to apply this hybrid as a catalyst for visible-light-driven CO2 reduction. In this hybrid photocatalytic system, the Ni(tpy) can provide specific catalytic sites and serve as electron sinks to suppress electron–hole recombination in the CsPbBr3 NCs. The CsPbBr3-Ni(tpy) catalytic system achieves a high yield (1724 μmol/g) in the reduction of CO2 to CO/CH4, which is approximately 26-fold higher than that achieved with the pristine CsPbBr3 NCs. This work has developed a method for enhancing the performance of photocatalytic CO2 reduction by immobilizing metal complexes on perovskite NCs. The methodology we present here provides a new platform for utilizing halide perovskite NCs for photocatalytic applications.
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ACS Applied Materials & Interfaces
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2020
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IF 8.758
Hai Zhu,Wenjun Lin,Qi Li,Yin Hu,Siyu Guo,Congmin Wang,Feng Yan
The exploitation of novel porous materials for capturing/adsorption of harmful gases is considered a very promising approach to deal with air pollution. Herein, bipyridinium-based ionic covalent triazine frameworks (ICTFs) were synthesized via ZnCl2-catalyzed ionothermal polymerization. The as-prepared ICTFs had a satisfactory total pore volume and specific surface of approximately 0.4582 cm3 g–1 and 1000 m2 g–1, respectively. Moreover, the specific surface area, pore size and distribution, and total pore volumes of ICTFs could be adjusted via ion-exchange of the anion. The obtained ICTFs were explored as the adsorbent for the separation/adsorption of the mixed gases (SO2, CO2, NO, and N2), and they showed the strong adsorption ability for CO2 (2.75 mmol g–1), SO2 (9.22 mmol g–1), and NO (4.05 mmol g–1) at 1 bar and 298 K. This unique design provides a new insight to prepare high-efficiency porous materials for CO2, SO2, and NO capture.
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Journal of CO2 Utilization
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2020
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IF 5.993
Bike Zhang,Mengchu Wang,Jiaqi Ding,Younan Li,Guanghan Cao,Matthew T. Bernards,Yi He,Yao Shi
The CO 2 electroreduction reaction (CO 2 ER) is a reliable pathway that enables a balanced carbon cycle for sustainable development strategies. There are several major challenges, such as selectivity , efficiency, and stability of the electrocatalysts that need to be addressed for the widespread application of this in the reduction of CO 2 . Herein, we develop an oxide-modification of Cu 1.81 S particles supported on multi-walled carbon nanotube (MWCNT) composites (Cu 1.81 S@WMCNT-600-OD) through a facile in-situ crystallization strategy. This modification improves the electroreduction activity in the reduction CO 2 to formate with a low onset-potential of -0.47 V vs RHE (overpotential = 0.25 V). In addition, the material used in preparing this catalyst is widely accessible at low cost. Among the electrocatalysts tested, Cu 1.81 S@WMCNT-600-OD exhibits a high CO 2 selectivity towards formate at an overpotential of 0.45 V with high faradaic efficiency (82 %) for nearly 20 h. Further investigations reveal that the needle-like dendritic structure formed during electrolysis is the likely source for the improved performance in CO 2 reduction. Therefore, this work provides low-cost, abundant, and efficient catalysts for CO 2 ER and a facile pathway that improves the electrocatalytic performance.
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LANGMUIR
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2020
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IF 3.557
An Chen,Xueyan Liu,Yuxin Wu,Guangsheng Luo,Jian-hong Xu
CO2-responsive switchable emulsions have been of great interest in some industrial processes where the stability of the emulsion is only required temporarily, such as oil transport, drug delivery, and fossil fuel production. The good understanding of the stability and instability mechanism is vital to the switchable behavior between emulsification and demulsification. Herein, a novel approach was developed to determine the interactions between two switchable emulsion droplets directly by a dual-laser optical tweezers instrument. The repulsive force between a couple of tetradecane droplets occurs to increase progressively with the increasing concentration of switchable surfactant in solutions. However, the repulsive force appears to decrease progressively in turn when the switchable surfactant concentration is far higher than the critical micelle concentration (CMC). Moreover, the depletion effect starts to emerge in the higher surfactant concentration which is attributed to the switchable surfactant micelles generated in solutions. In addition, according to the measurements of interaction forces, a mechanism of the switchable behavior is well proposed, which is established by the principle of self-assembly/detachment of the switchable surfactant, resulting in the weakening and re-enhancing of the electrostatic double-layer (EDL) repulsive forces between tetradecane droplets, upon selective introduction and removal of CO2. Based on this work, a novel perspective was provided to study the switchable emulsion, which can contribute instructive messages for the understanding of stability and instability mechanisms of switchable emulsions.
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Zheyuan Guo,Zihan Qu,Hong Wu,Rui Zhao,Yingzhen Wu,Yutao Liu,Leixin Yang,Yanxiong Ren,Chumei Ye,Zhongyi Jiang
Well-connected transport pathways play a critical role in high-performance CO2-facilitated separation membranes. Inspired by the ionic cluster network in polymer electrolyte membranes (PEMs) for fast ion transport, designing a unique CO2-philic cluster network structure is a promising strategy to construct efficient CO2 transport channels in membranes. Herein, a forced induction method is presented to construct a CO2-philic cluster network in membranes. Sulfobutylether-beta-cyclodextrin (sβ-CD) is introduced in a quaternary ammonium polysulfone (QAPSf) matrix. During the membrane formation process, the quaternary ammonium groups on QAPSf are attracted by the sulfonic acid groups on sβ-CD, assembling around and thus forming hybrid clusters. These clusters are swollen and interconnected by water under a humidified state. The hybrid cluster network acts as an effective CO2 transport pathway via clustering quaternary ammonium ion pairs as continuous CO2-facilitated transport sites. Simultaneously, the internal cavity of sβ-CD in hybrid clusters affords additional free volume in membranes, thus enhancing the CO2 permeability. The resultant QAPSf/sβ-CD membrane exhibits an optimal CO2 permeability of 1303 Barrer, a CO2/CH4 selectivity of 39, and good long-term operation stability for 30 days, surpassing the 2008 Robeson upper bound limit. This concept of constructing a hybrid cluster network for facilitated transport is expected to be applicable to explore more advanced PEMs for effective gas separation.
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NANOTECHNOLOGY
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2020
·Vol. 31
·期 21
·215605
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IF 3.551
Yu-Wei Liu,Shao-Hong Guo,Si-Qi You,Chun-Yi Sun,Xin-Long Wang,Liang Zhao,Zhong-Min Su
Halide perovskites have been employed as photocatalysts for CO2 photoreduction due to their excellent optical properties and unique electronic structure. However, their photocatalytic performance is relatively poor. Herein, we demonstrate a new strategy with Mn-doped CsPb(Br/Cl)3 mixed-halide perovskites as catalysts to enhance the efficiency of CO2 photoreduction. By tuning the content of Mn, a series of CsPb(Br/Cl)3:Mn perovskites are obtained and show high efficiency in CO2 conversion to CO and CH4. For the optimum catalyst sample, especially, the yields of CO and CH4 reach 1917 μmol g−1 and 82 μmol g−1 which are 14.2 and 1.4 times higher than those of CsPbBr3. This work provides new insights into improving the reactivity of perovskites in CO2 photoreduction.
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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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SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Li Wang,Jihe Zhao,Hongsheng Lu,Zhiyu Huang,Baogang Wang
In many practical processes, it is necessary to separate the aliphatic amine from the aromatic amine from water to obtain the desired product. A simple and effective strategy was proposed for selective separation of aliphatic amines from aromatic amines by using CO 2 . With the introduction of CO 2 into the aqueous solution, aliphatic amines can be switched from hydrophobicity to hydrophilicity but aromatic amines cannot due to their different p K a . The separation performance associated with product purity cannot be explained by p K a or log K ow . Thus, solubility parameter was employed to explain the separation performance of these amines. The relationship between solubility parameter and separation performance was investigated by gas chromatography and ultraviolet spectrophotometry , which established the concentration of each aliphatic amine in aromatic amine and that of aromatic amine in water. This relationship can guide the selection of appropriate switchable-hydrophilicity solvents (SHSs) to acquire better quality products. In addition, aliphatic amines dissolved in water could be regenerated by removing CO 2 and the recovery of aliphatic tertiary amines was up to 93.4%.
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JOURNAL OF CATALYSIS
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2020
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IF 7.888
Lan Yuan,Yue-Hua Li,Zi-Rong Tang,Jinlong Gong,Yi-Jun Xu
Pairing CO 2 reduction with oxidative organic synthesis in one photoredox cycle opens a new avenue for cooperative utilization of excited electrons and holes towards efficient solar-to-chemical energy conversion. In this work, we demonstrate a facile cetyltrimethylammonium bromide (CTAB) surfactant functionalized ZnIn 2 S 4 (ZIS)-based dual-functional reaction system for efficient visible light-driven CO 2 -to-CO conversion pairing with selective oxidation of benzyl alcohol to value-added C C coupled products. Our research suggests that the markedly enhanced redox activities are mainly attributed to the unique structure of CTAB-ZIS featuring more crystalline and surface defects, which greatly promotes the interfacial charge carrier transfer, and in particular elevates CO 2 activation and electrons reducibility. It is anticipated that this work would inspire further establishment of efficient novel photocatalysts and cooperative reaction system coupling CO 2 reduction and organic synthesis in a cost-effective manner under ambient conditions to meet the economic and social sustainability goals.
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