CARBON
·
2023
·
IF 10.9
Yuting Yin,Wenhao Jing,Feng Wang,Ya Liu,Liejin Guo
Coupling light absorber with an efficient cocatalyst is the most common way to fabricate composite photocatalyst . The light absorber supplies electrons and holes, while the cocatalyst domains chemical reactions. Inspired by the results from electrochemical CO 2 reduction, Cu-based materials are the most promising cocatalysts for photocatalytic CO 2 reduction. However, oxide-derived copper (OD-Cu) hasn't been introduced into photocatalytic systems yet, due to easily undergoing valence changes once exposed to air. Herein, we find that OD-Cu could be decorated on photocatalyst, polymeric C 3 N 4 (PCN), by a self-designed in-situ electroreduction method. The as-prepared OD-Cu/PCN presents better visible light absorption than the one without in-situ electroreduction and prefers multi-carbon products. According to CO 2 RR measurements, the highest selectivity to C 2 H 5 OH is 58%. Density functional theory calculation further indicates that the unique structure between OD-Cu and PCN leads to a low energy barrier of C–C coupling due to the enhanced *CO dimerization and thus promotes the production of C 2 H 5 OH. Moreover, this optimized sample achieves a solar-to-fuel efficiency, of up to 0.94%, which is 1.69 times the pristine PCN.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Hailong Liao,Heping Xie,Shuo Zhai,Ling Fu,Yuan Zhang,Senran Hao,Bin Chen,Chuanxin He,Zongping Shao
Aqueous Zn-CO 2 batteries are a new technology for reducing carbon dioxide emissions and converting CO 2 into valuable products. The development of high-performance catalysts is crucial for improving the efficiency of the CO 2 reduction reaction(CO 2 RR) in these batteries. The technical challenges of CO 2 RR catalysts include high cost, complicated synthesis and low Faraday efficiency. In this study, we developed an efficient and cost-effective CO 2 RR perovskite catalyst, by partially substituting Fe to the B site of precious metal-free La 0.5 Sr 0.5 MnO 3 (LSM) perovskite. Comprehensive investigation into the Structure, morphology, coordination information and electrochemical performance of pristine La 0.5 Sr 0.5 MnO 3 (LSM) and substituted La 0.5 Sr 0.5 Fe 0.6 MnO 3 (LSF 0.6 M) catalysts were conducted, LSF 0.6 M catalyst shows enhanced electrochemical performance, Faraday efficiency, battery durability and battery power density than LSM. Specifically, the Fe-doped catalyst shows a significant improvement in CO 2 reduction reaction (CO 2 RR) performance, with an 80% increase in current density, an 82% Faraday efficiency, and a 50% increase in power density of Zn-CO 2 battery. Characterization experimental results and DFT calculation reveal that Fe substitution can increase the perovskite lattice size to favor CO 2 absorption and *COOH formation, thus the improved CO yields. These analyses provided insights into the underlying mechanisms of the catalyst's performance in CO 2 RR within the battery system. These results highlight LSF 0.6 M perovskite as a very promising CO 2 RR electrocatalyst for Zn-CO 2 battery.
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PROGRESS IN ORGANIC COATINGS
·
2023
·
IF 6.6
Jiahui Chen,Yanyan Cui,Zhu Ding,Honggang Jiang,Zonglin He,Lina Song,Baohua Liu
Poly (propylene carbonate) diol with double-bonds on the side chains (PPCAGE) was synthesized form CO 2 , propylene oxide (PO), polyether diol (PPG) and allyl glycidyl ether (AGE). Then, three kinds of CO 2 based polyurethane oligomers (PPCAGE-PU) (PPCAGE-PUA, PPCAGE-PUB and PPCAGE-IPDI, respectively) with different contents of double bond were prepared through the reaction of PPCAGE, isophorone diisocyanate (IPDI) and hydroxyethyl acrylate (HEA). The content of -NCO was adjusted by varying the ratio of -NCO terminated prepolymer and HEA. Acrylate copolymer with side double bonds and hydroxyl groups (GMA-PSA) was synthesized by the ring-opening reaction of glycidyl methacrylate (GMA) and acrylate copolymer (PSA) containing -COOH and -OH. CO 2 based UV-induced peelable adhesive was prepared by mixing PPCAGE-PU, GMA-PSA, active diluent and photoinitiator. The structure of PPCAGE was confirmed by Fourier transform infrared (FT-IR) and nuclear magnetic resonance ( 1 H NMR). The reaction of PPCAGE-PUB and GMA-PSA was monitored by FT-IR, companied by the titration of -NCO and epoxide. The molecular weight of PSA and GMA-PSA was determined by gel permeation chromatography (GPC). The surface morphology of the adhesive was observed by scanning electron microscopy (SEM). The viscoelasticity of adhesive was measured by real-time rheology. The 180° peel strength , micro-surface morphology, gel content, unsaturation conversion and glass transition temperature of UV-induced peelable adhesive were characterized. The results showed that the peel strength of adhesive was 17.82 N/25 mm before UV curing. After UV curing, the surface morphology changed from smooth to rough, the peel strength decreased to 0.08 N/25 mm and the modulus of the PSA increased due to the cross-linking. DSC results showed that the glass transition temperature increased after UV curing.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Menglin Wu,Jiupai Ni,Chengsheng Ni
In situ exsolution of nanoparticles has been reported to be an efficient path to optimize CO2 electrolysis performance. Herein, a Ce/Co co-doped SrFeO3-δ (SF) can achieve the co-exsolution of CeO2 and Co–Fe alloy in 5% H2 at 800 °C. A small amount (<10%) of Ce-doped SF cannot stabilize the perovskite structure in a reducing atmosphere. Sr0.9Ce0.1Fe0.9Co0.1O3 (10Ce10CoF) and Sr0.95Ce0.05Fe0.9Co0.1O3 (5Ce10CoF) as symmetric electrodes of solid oxide electrolysis cells showed an excellent electrolysis performance at 800 °C for CO2 electrolysis. The current densities of the cells with 5Ce10CoF and 10Ce10CoF reached 0.98 and 1.30 A cm–2 under a bias of 1.3 V after a 48 h durability test for CO2 electrolysis, respectively, and the performance difference, however, may be due to CeO2 being more easily exsolved from the 10Ce10CoF lattice. We also investigated the role of the exsolved CeO2 and oxygen vacancy (VO) in determining the CO2 electrolysis performance via theoretical calculation. In this work, we designed a novel strategy to achieve the exsolution of CeO2 and Co–Fe alloy via reduction treatment and showed an outstanding CO2 electrolysis performance.
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CATALYSIS LETTERS
·
2023
·
IF 2.8
Ji Yaxiong,Lin Shuang,Xu Guihong,Chen Tianen,Gong Jianchao,Meng Fanbin,Wang Yuanhao
Abstract Catalytic conversion of CO 2 to methanol with H 2 from renewable energy has attracted increasing interest as a promising strategy for reducing excessive CO 2 emissions. However, the performance of reported various catalysts still suffers from low methanol yield with a passable CO 2 conversion. In this work, Cu–ZnO–La 2 O 3 interfaces are constructed with various La 2 O 3 mole ratio. Compared to Cu/ZnO, the optimized catalyst (i.e., Cu 0.6 Zn 0.2 La 0.4 ) exhibits a much higher mass-specific methanol formation rate (159.3 g MeOH /kg cat /h) at 240 °C and 3 MPa. A series of ex-situ and in-situ characterizations, such as X-ray diffractometer (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), N 2 O titration measurements, and in-situ diffuse reflectance Fourier transform infrared spectroscopy ( in-situ DRIFTS) study, are used to investigate its structure and mechanism study. The dispersion of Cu over Cu/ZnO/La 2 O 3 catalyst is significantly enhanced, forming more Cu–ZnO–La 2 O 3 interfaces. LaO x species favor CO 2 activation and generate more carbon intermediates species for CO 2 hydrogenation. Furthermore, more Cu + is bonded, which stabilizes the key intermediate, inhibits its desorption, and facilitates its further hydrogenation to methanol. This work is expected to offer an effective strategy to develop new catalysts with high performance for CO 2 hydrogenation to methanol. Graphical Abstract
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TRANSACTIONS OF TIANJIN UNIVERSITY
·
2023
·Vol. 29
·期 4
·293-303
·
IF 7.1
Liu Shengkun,Zhao Qiao,Han Xiaoxue,Wei Chongyang,Liang Haoting,Wang Yidan,Huang Shouying,Ma Xinbin
The interaction between a promoter and an active metal crucially impacts catalytic performance. Nowadays, the influence of promoter contents and species has been intensively considered. In this study, we investigate the effect of the iron (Fe)–zinc (Zn) proximity of Fe–Zn bimetallic catalysts on CO 2 hydrogenation performance. To eliminate the size effect, Fe 2 O 3 and ZnO nanoparticles with uniform size are first prepared by the thermal decomposition method. By changing the loading sequence or mixing method, a series of Fe–Zn bimetallic catalysts with different Fe–Zn distances are obtained. Combined with a series of characterization techniques and catalytic performances, Fe–Zn bimetallic proximity for compositions of Fe species is discussed. Furthermore, we observe that a smaller Fe–Zn distance inhibits the reduction and carburization of the Fe species and facilitates the oxidation of carbides. Appropriate proximity of Fe and Zn (i.e., Fe 1 Zn 1 -imp and Fe 1 Zn 1 -mix samples) results in a suitable ratio of the Fe 5 C 2 and Fe 3 O 4 phases, simultaneously promoting the reverse water–gas shift and Fischer–Tropsch synthesis reactions. This study provides insight into the proximity effect of bimetallic catalysts on CO 2 hydrogenation performance. Graphical Abstract
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ADVANCED MATERIALS
·
2023
·Vol. 35
·期 33
·2302325
·
IF 29.4
Chang Guo,Fuli Zhang,Xiao Han,Lipeng Zhang,Qian Hou,Lele Gong,Jincheng Wang,Zhenhai Xia,Jianhua Hao,Keyu Xie
To date, the effect of noble metal (NM) electronic structures on CO 2 reaction activity remains unknown, and explicit screening criteria are still lacking for designing highly efficient catalysts in CO 2 -breathing batteries. Herein, by preferentially considering the decomposition of key intermediate Li 2 CO 3 , an intrinsic descriptor constituted of the d x 2 − y 2 ${{\rm{d}}}_{{x}^2 - {y}^2}$ orbital states and the electronegativity for predicting high-performance cathode material are discovered. As a demonstration, a series of graphene-supported noble metals (NM@G) as cathodes are fabricated via a fast laser scribing technique. Consistent with the preliminary prediction, Pd@G exhibits an ultralow overpotential (0.41 V), along with superior cycling performance up to 1400 h. Moreover, the overall thermodynamic reaction pathways on NM@G confirm the reliability of the established intrinsic descriptor. This basic finding of the relationship between the electronic properties of noble metal cathodes and the performance of Li-CO 2 batteries provides a novel avenue for designing remarkably efficient cathode materials for metal-CO 2 batteries.
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PubMed
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Materials Chemistry Frontiers
·
2023
·Vol. 7
·期 16
·3382-3389
·
IF 7
Gaoming Sun,Chong Zou,Wen Sun,Ying Fang,Shuijian He,Yana Liu,Jiguang Zhang,Yunfeng Zhu,Jun Wang
The electrochemical reduction of CO2 to value-added products represents a promising strategy to store renewable energy and realize global carbon neutrality. Bi-based materials have attracted extensive attention for formate production from CO2 reduction. Herein, we employ BiPbO2Br nanosheets as the bimetallic oxyhalide precursor to prepare a reconstructed Bi–Pb composite catalyst by electroreduction. The resultant catalyst exhibits impressive performance for formate production, including a high partial current density (40 mA cm−2 at −1.0 V), a high faradaic efficiency (96.6% at −0.9 V), a high energy conversion efficiency (>50% from −0.8 to −1.1 V), and good stability. As compared with the monometallic Bi and Pb counterparts, the Bi–Pb composite catalyst demonstrates superior intrinsic performance, which is attributed to the multiphase composites and abundant heterogeneous interfaces derived from electroreduction induced structural reconstruction of BiPbO2Br. This work offers an attractive strategy to further improve the performance of Bi catalysts for CO2 reduction to formate.
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Small
·
2023
·Vol. 19
·期 40
·2303099
·
IF 13.3
Zi Yang,Deguang Ji,Zhi Li,Zidong He,Yang Hu,Jie Yin,Yichao Hou,Pinxian Xi,Chun-Hua Yan
Copper-based electrocatalysts effectively produce multicarbon (C 2+ ) compounds during the electrochemical CO 2 reduction (CO 2 RR). However, big challenges still remain because of the chemically unstable active sites. Here, cerium is used as a self-sacrificing agent to stabilize the Cu + of CuS, due to the facile Ce 3+ /Ce 4+ redox. CeO 2 -modified CuS nanoplates achieve high ethanol selectivity, with FE up to 54% and FE C2+ ≈ 75% in a flow cell. Moreover, in situ Raman spectroscopy and in situ Fourier-transform infrared spectroscopy indicate that the stable Cu + species promote C C coupling step under CO 2 RR. Density functional theory calculations further reveal that the stronger * CO adsorption and lower C C coupling energy, which is conducive to the selective generation of ethanol products. This work provides a facile strategy to convert CO 2 into ethanol by retaining Cu + species.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Lin Yan,Wang Tuo,Zhang Lili,Zhang Gong,Li Lulu,Chang Qingfeng,Pang Zifan,Gao Hui,Huang Kai,Zhang Peng,Zhao Zhi-Jian,Pei Chunlei,Gong Jinlong
The mechanism of how interfacial wettability impacts the CO 2 electroreduction pathways to ethylene and ethanol remains unclear. This paper describes the design and realization of controllable equilibrium of kinetic-controlled *CO and *H via modifying alkanethiols with different alkyl chain lengths to reveal its contribution to ethylene and ethanol pathways. Characterization and simulation reveal that the mass transport of CO 2 and H 2 O is related with interfacial wettability, which may result in the variation of kinetic-controlled *CO and *H ratio, which affects ethylene and ethanol pathways. Through modulating the hydrophilic interface to superhydrophobic interface, the reaction limitation shifts from insufficient supply of kinetic-controlled *CO to that of *H. The ethanol to ethylene ratio can be continuously tailored in a wide range from 0.9 to 1.92, with remarkable Faradaic efficiencies toward ethanol and multi-carbon (C 2+ ) products up to 53.7% and 86.1%, respectively. A C 2+ Faradaic efficiency of 80.3% can be achieved with a high C 2+ partial current density of 321 mA cm −2 , which is among the highest selectivity at such current densities.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yubin Wang,Zifei Yan,Jian Deng,Guangsheng Luo
Microdevices are becoming a hot technology for process intensification of CO 2 capture. However, most microdevices are limited to a small handling capacity, low volume gas to liquid ratio, and cocurrent flow mode. In this context, we proposed a miniaturized annular rotating device ( m -ARD), which has a high handling capacity, can be employed for high volume ratios of gas to liquid, and utilizes a countercurrent flow mode. Variables were investigated to determine the flow characteristic, absorption efficiency of CO 2 , and volume mass transfer coefficient. The gas hold-up and specific surface area in the m -ARD were up to 43.8 % and 1000 m 2 /m 3 , and low pressure drop was observed. Notably, the optimal volume gas to liquid phase ratio, absorption efficiency of CO 2 , and overall volumetric mass transfer coefficient were close to 200 %, 100 %, and 0.53 s −1 , respectively. Furthermore, two dimensionless equations were built to predict the volumetric mass transfer coefficient and gas hold-up. In addition, the contributions of the specific surface area and mass transfer coefficient for enhancing CO 2 absorption were discussed, respectively. This work provides a prospective device for enhancing CO 2 capture and other gas–liquid separation and reaction processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Meng Yang,Shujuan Wang,Lizhen Xu
Water vapor in air significantly affects the CO 2 separation performance of solid amine sorbents. Although moisture benefits the CO 2 adsorption process, the co-adsorbed H 2 O in amine sorbents leads to extra regeneration energy consumption, which challenges the application of solid amine sorbents for direct air capture. Reducing H 2 O adsorption and improving the CO 2 /H 2 O selectivity of solid amine sorbents are fundamental solutions. This work clarified the more prominent hydrophilic contribution of polyethylenimine (PEI) layers than support resins for amine-impregnated sorbents. Then, we identified the phenyl group as the preferred additive to enhance the hydrophobic properties of PEI-impregnated sorbents using an orthogonal test. The introduction of hydrophobic phenyl groups reduced the average water vapor adsorption per amine group by more than 50% and increased the CO 2 /H 2 O selectivity of the amine resin sorbents by 68%–89%, resulting in lower heat requirement caused by H 2 O desorption. Despite the modification reduced CO 2 uptake, a modest CO 2 capacity of 1.47–1.6 mmol/g was detected of BZ13.5–40%R20 in a representative air condition (28 °C, relative humidity 50%). In addition, BZ13.5–40%R20 showed stable CO 2 capacity in 10 consecutive temperature swing adsorption cycles (desorption at 70 °C, N 2 stripping) in laboratory.
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