ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Xiaofeng Lai,Song Wang,Ying Xie,Binghang Liu,Jianhui Sun,Yuxin Li,Haitao Yu,Kai Pan
CsPbBr3 perovskite nanocrystals have emerged as promising candidates for photocatalysis. However, their conversion efficiency is hampered by material instability, and the accumulation of deactivated perovskites produced after photocatalytic reactions raises significant environmental concerns. To address this issue, we developed a mechanochemical grinding approach assisted by oleylamine as an additive to restore the optical properties and photocatalytic activity of deactivated CsPbBr3, which was due to aggregation in the photocatalytic CO2 reduction reaction. Upon regeneration, the CsPbBr3 nanocrystals exhibited an average length of 34.21 nm and an average width of 20.86 nm, demonstrating optical properties comparable to those of the pristine CsPbBr3 nanocrystals. Moreover, they achieved a conversion efficiency of 88.7% compared with pristine CsPbBr3 nanocrystals in the photocatalytic CO2 reduction reaction. This method effectively enhanced the utilization of CsPbBr3, offering a novel approach for the recycling and recovery of perovskite materials and thereby minimizing material waste and environmental pollution.
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Surfaces and Interfaces
·
2023
·
IF 6.2
Ning Liu,Bin Hu,Kexin Tang,Tingyu Xia,Fei Li,Guixiang Quan,Xiaodong Zhang,Liang Tang
In the pursuit of restoring and preserving our planet's natural equilibrium, the development of photocatalytic agents with exceptional aptitude for CO 2 reduction stands as an essential undertaking, which would be greatly facilitated with the energy regeneration and environmental purification. Herein, a composite material HTiNbO 5 /UiO-66 (UTi) was amalgamated by a one-step solvothermal method. The resultant composite material exhibited remarkable improvement on the photoreduction efficiency of CO 2 reduction compared with pristine UiO-66 and HTiNbO 5 . Impressively, UTi composite with 3 wt% HTiNbO 5 (UTi-3) illustrated the highest CO 2 photoreducation activity to CO, the CO yield of UTi-3 was about 9.3 and 11.2 times higher than that of pure UiO-66 and HTiNbO 5 , respectively. The significantly improved photocatalytic performance could be ascribed to the enlargement of specific surface area, the improved visible-light absorption range and shrinkage of the energy band gap, which can increase photogenerated electron production to promote the reduction reaction of CO 2 to CO. The insights obtained from this study can guide the application of semiconductor composites in the field of CO 2 photocatalytic reduction, so as to design high efficiency photocatalysts .
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Gels
·
2023
·Vol. 9
·期 9
·703
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IF 4.6
Kaibo Xu,Liqin Cao
Herein, a green, carbon dioxide-in-water high-internal-phase emulsion (C/W HIPEs) was developed and stabilized with polyvinyl alcohol (PVA) for the formation of chitosan oligosaccharide/poly(acrylamide-co-sodium 4-styrene sulfonate) [COS/P(AM-co-SSS)] monolithic porous hydrogel. The obtained monolith was characterized via FT-IR and SEM. The SEM patterns depicted that the monoliths were interconnected, the void sizes were 78.5 µm, and the interconnected pore throats were 28 μm approximately. Mechanical measurement results indicated that the maximum compress stress of the monolith could reach 334.4 kPa at 90% strain, and it exhibited good mechanical stability. After 200 cycles of compression, it could still recover its original shape without cracking. The obtained COS-based monolith was selected to remove tetracycline (TC) for evaluating the adsorptive features of the interpenetrating pore-containing monolith. The monolithic COS/P(AM-co-SSS) hydrogel behaved with strong antibiotic adsorption capacity (1600.4 mg/g for TC). The adsorption process agreed well with the pseudo-second-order kinetic and Langmuir isothermal models. In addition, the porous monolith had a strong electrostatic force on TC according to the thermodynamic study. This work provides a green route for the development of novel monolithic hydrogels and highlights its potential application in the treatment of antibiotic-containing wastewater.Keywords:high-internal-phase emulsion;CO2-in-water;chitosan oligosaccharides;monolith;porous;hydrogel
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Chao Miao,Kaixuan Shang,Lixing Liang,Shumei Chen,Jing Ouyang
In this work, a Ni-based catalyst supported on a core–shell structure catalytic carrier material (Ni/ZSM-5@MCM-41) based on kaolinite tailings is reported, which exhibits excellent CO2 methanation performance at atmospheric pressure. At 400 °C, CO2 conversion and CH4 selectivity reach 80 and 97% with the space velocity of 12,000 mL gcat–1 h–1, respectively, and it can maintain good stability during the 80 h stability test. Compared with traditional Ni/ZSM-5 and Ni/MCM-41 catalysts, Ni/ZSM-5@MCM-41 has more substantial confinement effects on the active components, and the active components are more evenly dispersed on surface of the carrier. In addition, it is confirmed by the in situ diffuse reflectance infrared Fourier transform spectroscopy technique that CO2 methanation over the Ni/ZSM-5@MCM-41 catalyst follows the path of formate and CO as intermediates.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Guanzhang Liu,Hang Yuan,Xiaobo Li,Ke Li,Lei Mao,Guangya Zhang
Carbon dioxide capture, conversion, and utilization with carbonic anhydrase (CA) as a green and sustainable method still faces the challenges of complex and costly purification, relatively low yield, and poor catalytic performances and reusability. Herein, we proposed an all-in-one strategy to solve these problems by self-assembling nanosized CA oligomeric particles (nCAOPs) into micrometer-sized CA supraparticles (mCASPs) with well-designed tags. The preparation of the purified mCASPs was simple and effective by an easy scalable low-speed centrifugation method with 78% activity recovery. The obtained mCASPs with a yield of 870 mg/L was the reported highest yield of CAs. Interestingly, mCASPs could serve as carrier-free immobilized CAs and retain over 90% original activity after 15 reuse cycles. More encouragingly, mCASPs could redissolve and form nCAOPs, which had excellent catalytic performances. The hydrated activity of nCAOPs was 1.05 times that of free CAs. Also, the kcat/Km value was 1.74 times that of free CAs, and the half-life at 40 °C was 3.83 times that of free CAs. Due to the simplicity of purification and immobilization, high yield, and excellent enzymatic properties, mCASPs and nCAOPs are considered novel bioactive materials, which offer the feasibility of CAs for sustainable CO2 capture to achieve the target of carbon neutrality.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Meisi Chen,Mengjia Li,Lin Zhang,Xiemin Liu,Feng Zhang,Youting Wu
Amino acid ionic liquids (AAILs) exhibit prominent merits for CO2 capture including biocompatibility and good stability, but they still suffer from several demerits, such as high viscosity and low molecular utilization. Therefore, it is critical to construct proper systems that can address these problems to enhance CO2 absorption of AAILs. In this work, three types of AAIL absorbent systems, DMEE (2-[2-(dimethylamino) ethoxy] ethanol)–AAIL, H2O–AAIL, and EG (ethylene glycol)–AAIL, are prepared with six AAILs that have different amino acids. The absorption performance of these absorbents is characterized to investigate the reinforcing effects of the additives on the absorption properties of AAILs. With temperatures ranging from 293 to 313 K, the CO2 capture studies on the binary systems reveal that AAILs present better absorption efficiency when their concentrations are 40 or 50 wt %. Based on the zwitterion reaction mechanism model and a thermodynamic model, the interactions of AAILs with H2O, DMEE, and EG systems for absorbing CO2 are discussed, respectively. The results obtained in this work indicate that AAIL–DMEE systems are promising candidates for CO2 capture since the interaction between AAILs and DMEE increases the capacity of AAILs and promotes kinetics.
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ACS Catalysis
·
2022
·
IF 13.7
Xiwen Song,Chengsheng Yang,Xianghong Li,Zhongyan Wang,Chunlei Pei,Zhi-Jian Zhao,Jinlong Gong
Understanding the nature of adsorbates and intermediates on catalytic surfaces is critical for the development of highly efficient systems for CO2 conversion. However, the role of structural hydroxyl groups in CO2 hydrogenation is still under debate. This paper describes an experimental study on the nature of surface-bound hydroxyl groups over Al2O3-supported Cu catalysts for CO2 reduction. A model 5 wt % Cu/Al2O3 catalyst with stable hydroxyl groups was prepared. The structural hydroxyl groups were modulated by the hydration of unsaturated Al3+ sites, which were introduced by the evaporation-induced self-assembly method. Terminal hydroxyl groups (T-OH*) were found to significantly facilitate the conversion of CO2, while the AlVI-T-OH and AlIV-T-OH species promoted the formation of Al-b-HCOO and Al-m-HCOO species, respectively, accompanied with the increase in methanol and dimethyl ether yields. The reaction behavior of hydroxyl species was further investigated by in situ IR experiments with HD isotope exchange on Cu/Al2O3. T-OH* were identified as active sites participating in the formation of key intermediates, while more hydroxyl sites were occupied by formate species with the H coadsorbed on the Cu surfaces.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Jinchang Liu,Yaping Li,Xiaoya An,Chenyang Shen,Qiang Xie,Dingcheng Liang
Wasted coal liquefaction residual was used to synthesize activated carbon fibers (ACFs) for CO 2 capture, and the properties of the developed ACFs were optimized by adjusting the activation conditions, including the reaction temperature and soaking time. The yield, element distribution, pore structure, composition, functional group, morphology, and adsorption capacity of the as-synthesized ACFs were characterized by various apparatuses. In addition, static and dynamic adsorption experiments were conducted to investigate the adsorption capacity of CO 2 in flue gas . The results revealed that the synthesized ACFs are mainly composed of carbon, accounting for more than 90% of the total elements. The specific surface area, pore volume, and pore width distribution of the prepared ACFs were optimized by changing the activation conditions, and ACFs with a specific surface area higher than 1400 m 2 /g were successfully developed by activation at 950 for 3 h. The amount of micropores occupied more than 90% of the total pore volume. The pore width distribution dominated by micropores is beneficial for CO2 adsorption since the diameter of CO 2 is 0.33 nm. From FTIR and XPS analysis, it is found that the main structure of ACFs is a carbon skeleton composed of polycyclic aromatic hydrocarbons with a small number of oxygen-containing functional groups. The adsorption isotherm of ACFs for CO 2 conforms to the Langmuir model, indicating that the adsorption process of CO 2 by ACFs can be attributed to monolayer adsorption. Both the specific surface area and oxygen-containing functional groups have crucial effects on the adsorption capacity of CO 2 . The dynamic adsorption experiment determined that ACFs-920-3 had the highest adsorption capacity for CO 2 in flue gas, and adsorption equilibrium was achieved after 7 min of adsorption. The adsorption process of CO 2 in flue gas by the as-synthesized ACFs fits well with the pseudosecond kinetic model. The CO 2 adsorption capacity of the obtained ACFs remained unchanged after 10 cycles of adsorption. A high-value-added route for synthesizing ACFs for CO 2 capture using CLR as a raw material was developed.
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CARBOHYDRATE POLYMERS
·
2022
·
IF 10.723
Yi Sun,Wei Zhang,Shan Lu,Wenhua Miao,Meiling Chen,Fei Liu,Haining Na,Jin Zhu
Herein, a novel cellulose-based fluorescent material with amine-responsive property was developed in a CO 2 switchable solvent for the contactless, real-time, and visual monitoring of the freshness of shrimp , crab, and fish. A nucleophilic cellulose carbonate intermediate is in-situ formed upon dissolution of cellulose in the CO 2 switchable solvent, which is adopted for the highly effective grafting of poly( l -lactic acid) and amine-responsive fluorescent reagent 7-amino-4-(trifluoromethyl) coumarin onto the cellulose backbone via ring opening polymerization and nucleophilic substitution reaction, respectively. The product has good processibility, and sensitive and reversible fluorescent responsive towards ammonia. The fluorescent intensity of the material decreased significantly and its fluorescent color changed from blue to cyan, when the aquatic products got spoiled. This study indicates that the CO 2 switchable solvent has great potential for the modification of cellulose with various functionality by taking advantage of the highly active nucleophilic cellulose carbonate intermediate.
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RSC Advances
·
2022
·Vol. 12
·期 40
·26307-26318
·
IF 4.036
Juan Bai,Ziwei Song,Lijuan Liu,Xu Zhu,Faming Gao,Raghunath V. Chaudhari
Metal–organic frameworks (MOF) have been studied extensively for the adsorption and catalytic conversion of CO2. However, previous studies mainly focused on the adsorption capabilities of partially or totally Ce substituted UiO-66, there are few studies focusing on transformation of the structure and catalytic activity of these materials. In this work, a series of Zr/Ce-based MOFs with UiO-66 architecture catalysts were prepared for the conversion of CO2 into value-added dimethyl carbonate (DMC). Owing to the different addition order of the two metals, significantly varied shapes and sizes were observed. Accordingly, the catalytic activity is greatly varied by adding a second metal. The different catalytic activities may arise from the different acid–base properties after Ce doping as well as the morphology and shape changes. Besides, the formation of terminal methoxy (t-OCH3) was found to be the rate limiting step. Finally, the reaction mechanism of CO2 transformation in the presence of a dehydrating agent was proposed.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 44
·17081-17088
·
IF 4.569
Wenyuan Wang,Kai Zhang,Tao Xu,Yagang Yao
Nowadays, the goal of carbon peaking and carbon neutrality has become a global consensus, and electrochemical CO2 reduction to provide high-value power fuel is one of the major technical approaches attracting significant research interests and application prospects. However, the inevitable hydrogen evolution reaction in water-based electrolyte systems crowds out the reactive sites of active metals, causing a low CO2 conversion efficiency. In this work, Zn nanosheets were prepared via electrodeposition on the surface of carbon paper and then modified with polytetrafluoroethylene (PTFE) to tune the wetting angle of the electrolyte. A CO faradaic efficiency of 90.2% was achieved for Zn NS-8% PTFE (contact angle: 136.8°) at the electrolytic voltage of −1.0 V vs. RHE along with an overall current density of −7.9 mA cm−2. Experimental results and molecular dynamics simulation revealed that PTFE weakened the aggregation of H2O molecules and was more beneficial for capturing and adsorbing CO2 molecules near the electrode surface. The active sites of hydrogen production were transformed into the reaction center for electrocatalytic CO2 reduction due to the hydrophobicity of the electrode, and the accumulation of the local CO2 concentration accelerated the kinetic activity for electrochemical conversion (CO2 to CO). This strategy of tuning the local environment offers an alternative approach for effective electrode manufacturing in liquid electrolytes.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Yimeng Zhou,Qianjin Ye,Xiangli Shi,Qiong Zhang,Qi Song,Changjian Zhou,Di Li,Deli Jiang
Due to the multiple electron and proton transfer processes involved, the photogenerated charges are easily recombined during the photocatalytic reduction of CO2, making the generation of the eight-electron product CH4 kinetically more difficult. Herein, Ni3B nanoparticles modulated by p-block element were combined with TiO2 nanosheets to construct a novel Schottky junction photocatalyst (Ni3B/TiO2) for the selective photocatalytic conversion of CO2 to CH4. The formed Ni3B/TiO2 photocatalyst with Schottky junction ensures a transfer pathway of photogenerated electrons from TiO2 to Ni3B, which facilitates the accumulation of electrons on the surface of Ni3B and subsequently improves the activity of photocatalytic CO2 reduction to CH4. The optimized Ni3B/TiO2 Schottky junction shows an improved CH4 yield of 30.03 μmol g–1 h–1, which was much higher than those of TiO2 (1.62 μmol g–1 h–1), NiO/TiO2 (2.44 μmol g–1 h–1), and Ni/TiO2 (4.3 μmol g–1 h–1). This work demonstrated that the introduction of p-block elements can alleviate the scaling relationship effect of pure metal cocatalysts to a certain extent, and the modified Ni3B can be used as a promising new cocatalyst to effectively improve the selective photocatalytic of CO2 to CH4.
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