CARBON
·
2023
·
IF 10.9
Ruijia Wang,Jianyong Wan,Hongda Guo,Bing Tian,Shujun Li,Jian Li,Shouxin Liu,Tony D. James,Zhijun Chen
Converting CO 2 with various epoxides to cyclic carbonates is extremely important. However, most of catalysts for such conversion either require complicated fabrication or are obtained from unsustainable sources. Motivated by this problem, we prepare biomass-based “all-in-one” carbon dots as nano-organocatalysts for firstly converting CO 2 to cyclic carbonates. In this work, carbon dots (CD@KI) with high catalytic performance and good recyclability are prepared from sodium phytate (SP), polyethylenimine (PEI) and KI using one-pot hydrothermal treatment featuring cheap precursors and simple operation. Assisted by highly catalytic activity of CD@KI, up to 99.5% yield is achieved for converting CO 2 and various epoxides to cyclic carbonates under mild conditions (solvent-free and 1 atm of CO 2 ). Moreover, the conversion yield is maintained for reactions up to 10 g in scale. Significantly, by taking advantage of the inherent luminescence of CD@KI, the as-formed cyclic carbonates catalysed by CD@KI can be directly converted to afterglow polymer composites .
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ACS ES&T Engineering
·
2023
·
IF 7.1
Peng Chen,Yun Wang,Jiazhen Liao,Yi Liang,Qingqing Ye,Yi Wang,Zhongwei Jiang,Chunhui Shan,Wendong Zhang,Fan Dong
The dissociation of H2O molecules plays an important role in producing protons for promoting hydrogenation reduction of CO2. Therefore, developing excellent photocatalysts to promote the dissociation of H2O molecules and reveal the effect mechanism is the key research direction to enhance CO2 reduction efficiency. In this work, we synthesized BiSbO4 with oxygen vacancies (OVs) to investigate the photocatalytic mechanism of CO2 conversion and H2O dissociation. Experimental results indicate that the introduction of OVs into BiSbO4 can enhance the absorption capacity of light, narrowing band gaps and impeding the recombination of photogenerated carriers. Importantly, the existence of OVs in BiSbO4 can promote the adsorption and activation of H2O molecules via the stronger covalent interaction, which facilitates the dissociation of H2O molecules to generate more protons and lowers the energy barriers of •COOH to improve the efficiency of CO2 reduction. This study reinforces our understanding of the principle of photocatalytic CO2 reduction and the important role of H2O dissociation in photocatalytic CO2 conversion.
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Energy Technology
·
2023
·Vol. 11
·期 8
·2300119
·
IF 3.8
Shiyuan Liu,Ce Zhang,Wei Yao
Electrochemical CO 2 $\left(\text{CO}\right)_{2}$ reduction reaction is considered as a promising technical route for carbon-neutral and mitigating greenhouse effect. CO 2 $\left(\text{CO}\right)_{2}$ concentration limitation hinders the performance of state-of-the-art electrochemical CO 2 $\left(\text{CO}\right)_{2}$ reduction reaction. Increasing the mass transfer of reactants on the catalyst surface by flow cell design and porous electrode design has become the mainstream approach. Studying the distribution of mass in reaction region is important and beneficial to optimizing and designing efficient reactors. Herein, electrochemical CO 2 $\left(\text{CO}\right)_{2}$ reduction reaction reactors with micrometer and millimeter channels are simulated and systemically analyzed. The results reveal the microfluidic design can improve the mass transfer and reactant gas flow in the porous layer to reduce the concentration polarization and ensure uniform local potential of the reactor. A micrometer channel model requires only 10 sccm inlet gas supply to achieve the same current density compared to a millimeter flow channel with an inlet flow of 20 sccm. This study proposes a reasonable flow channel reactor to reduce gas stagnant region, which not only enhances the CO 2 $\left(\text{CO}\right)_{2}$ reduction performance effectively with evident potential dependence, but also guides the design for large-scale reactors.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Zhou Min,Wang Zhiqing,Mei Aohan,Yang Zifan,Chen Wen,Ou Siyong,Wang Shengyao,Chen Keqiang,Reiss Peter,Qi Kun,Ma Jingyuan,Liu Yueli
The precise construction of photocatalysts with diatomic sites that simultaneously foster light absorption and catalytic activity is a formidable challenge, as both processes follow distinct pathways. Herein, an electrostatically driven self-assembly approach is used, where phenanthroline is used to synthesize bifunctional LaNi sites within covalent organic framework. The La and Ni site acts as optically and catalytically active center for photocarriers generation and highly selective CO 2 -to-CO reduction, respectively. Theory calculations and in-situ characterization reveal the directional charge transfer between La-Ni double-atomic sites, leading to decreased reaction energy barriers of *COOH intermediate and enhanced CO 2 -to-CO conversion. As a result, without any additional photosensitizers, a 15.2 times enhancement of the CO 2 reduction rate (605.8 μmol·g −1 ·h −1 ) over that of a benchmark covalent organic framework colloid (39.9 μmol·g −1 ·h −1 ) and improved CO selectivity (98.2%) are achieved. This work presents a potential strategy for integrating optically and catalytically active centers to enhance photocatalytic CO 2 reduction.
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PubMed
高影响因子
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Zesheng Deng,Jiazhen Cao,Songchang Hu,Shiqun Wu,Mingyang Xing,Jinlong Zhang
CO2 photoreduction is considered one of the potential ways to achieve carbon neutralization since it uses green solar energy without introducing additional carbon sources during the process of converting CO2 to fuels. However, limited light utilization and poor charge separation often give rise to undesirable CO2 photoreduction performance. Herein, a generic approach using carbon spheres as templates to construct transition metal oxides with multishelled hollow structures is reported. The multishelled hollow structure has been proven to be efficient for improving CO2 photoreduction. Furthermore, we constructed a Z-scheme heterojunction photocatalyst (CdS/Au/ZnCrO4) through introducing CdS into a multishelled hollow ZnCrO4 sphere with Au nanoparticles as a charge transfer medium. Benefiting from the multishelled hollow structure’s induced light utilization and large surface area and Z-scheme heterojuncion promoted charge separation, a high CO production of 2.95 μmol g–1 h–1 was achieved on CdS/Au/ZnCrO4 without using any sacrificial agents, which was 18.4 times and 24.6 times higher than that of CdS and ZnCrO4. This work provides a generic method for constructing controllable multishelled hollow spheres and is expected to offer guidance for promoting CO2 photoreduction through structure regulation and heterojunction construction.
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Journal of CO2 Utilization
·
2021
·
IF 7.132
Tianbo Zhou,Yuxue Wang,Huanda Zheng,Bing Du,Laijiu Zheng
Traditional water medium dyeing of polyester-cotton fabrics consumes more water and energy, and causes serious environmental pollution in comparison with one-bath dyeing of single component fiber. To achieve sustainable dyeing of polyester-cotton blends, three reactive disperse dyes with s-triazine reactive group were synthesized, and supercritical CO 2 was used as solvent to conduct the waterless dyeing. The results showed that one-bath dyeing of polyester-cotton blends could be successfully realized with the synthesized dyes. Dyeing performance of the synthesized dyes was constantly improved with the extension of carbon chain on aniline. Compared with other two dyes, the optimal color strength of polyester-cotton blends was obtained with dye 3 using dimethylsulfoxide as co-solvent, and K/S values up to 6.4 were obtained at 100 °C, 20 MPa and 120 min with a dimethylsulfoxide concentration of 80 %. σ K/S values below 0.14 and washing and rubbing fastness above 4 were displayed for the colored samples. In addition, dyeing mechanism of polyester-cotton fabrics with the synthesized dyes was discussed combined with FT-IR measurement and stripping experiments.
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Catalysis Science & Technology
·
2021
·Vol. 12
·期 2
·606-612
·
IF 6.119
Yuqing Shao,Zhaolin Dou,Xiaoyu Liang,Xinxin Zhang,Min Ji,Min Pang,Min Wang,Xinkui Wang
The photocatalytic reduction of CO2 into valuable fuels and sustainable energy has a promising future, yet remains a challenge due to low charge separation efficiency and inadequate active sites. We find that ZnIn2S4-loaded secondary amine-functionalized organic silica (ZnIn2S4/NH–SiO2) was effective for visible-light driven CO2 photocatalytic reduction. The ZnIn2S4/NH–SiO2 with 40% ZnIn2S4 content achieves a CO production rate of 1304.8 μmol g−1 h−1 at room temperature, which is about 3 times higher than that of pristine ZnIn2S4. The thin ZnIn2S4 nanosheet accelerates the separation of photogenerated electron pairs, and the amine groups on ZnIn2S4/NH–SiO2 act as active sites for adsorption and activation of CO2, hence facilitating the photoreduction of CO2.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Shupanxiang Chen,Bo Jia,Yu Peng,Xiao Luo,Yangqiang Huang,Bo Jin,Hongxia Gao,Zhiwu Liang,Xiayi Hu,Yefeng Zhou
In this study, attapulgite (AT) was treated by high-temperature roasting and hydrochloric acid to form HcAT. It was then modified with 3-aminopropyltrimethoxysilane (APS) through the grafting method to synthesize a new adsorbent, which exhibits relatively low regenerative energy consumption in CO2 adsorption and desorption processes. Scanning electron microscopy (SEM), N2 adsorption–desorption, Fourier transform infrared spectroscopy, X-ray diffraction, and thermogravimetric analysis were selected to support the research. The CO2 adsorption process on the adsorbent was studied at different APS loadings and different temperatures. The maximal amount of CO2 adsorbed on the adsorbent is 1.81 mmol/g at 313 K when the APS mass fraction is 30%. The Freundlich isotherm model shows a great correlation with the CO2 adsorption isotherm obtained from the experimental data, and R2 reached up to 0.996. The isosteric heat while CO2 adsorbed on 30%APS-HcAT is calculated as 62.63 kJ/mol. The regeneration cyclic stability of 30%APS-HcAT is excellent, while the CO2 adsorption capacity only decreased by 3.2% after 10 cycles. The energy consumption in the CO2 desorption process was also calculated as 26.875 kJ/mol. Three different kinetic models were selected to fit the experimental data, and two models showed a great fit, which were the pseudo-second and Avrami’s fractional order models. The activation energy of 30%APS-HcAT was 38.826 kJ/mol, which can be calculated from the experimental data, and this value is higher compared with those of the other sorbents modified by the impregnation method and also much lower than the value of the chemical absorption process between traditional amine solvents and CO2.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Quan Shi,Ming-Hui Chen,Ji Xiong,Ting Li,Ya-Qing Feng,Bao Zhang
2D metal − organic framework (MOF) nanosheets have been demonstrated to exhibit excellent properties and prospects in various aspects, especially in photocatalysis . However, the design and direct preparation of 2D MOF photocatalyst is highly desirable but still challenging. Herein, a novel 2D porphyrin-based MOF Fe-DBP(Co), which is assembled by dicarboxylic porphyrin ligands and the unprecedented undecametallic ferric-oxo clusters, is designed and developed. The unique nanosheet morphology and assembled layered structure endows the photocatalyst with higher electron-hole separation efficiency and longer photogenerated carrier lifetime compared to the analogous MOFs. Consequently, Fe-DBP(Co) exhibits strikingly excellent and stable photocatalytic performance in CO 2 cycloaddition, and the reaction rate of 103.2 mmol∙g −1 ∙h −1 is among the state-of-the-art cases for MOF-photocatalyzed CO 2 cycloaddition. The underlying mechanism investigation suggested that photogenerated electrons transferred from CoDBP ligands to the Fe clusters, and the abundant electrons and holes promoted the generation of Fe(II) and Co(III) respectively, leading to excellent catalytic performance. This work proposes a new strategy to design and develop efficient MOF photocatalysts for photocatalytic transformation of CO 2 .
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ENERGY & FUELS
·
2023
·
IF 5.3
Linghan Xia,Mengchen Wu,Yimeng Li,Hongyan Guo,Yonghong Cheng,Guodong Meng
As one of the most consensus goals around the world, reduction of carbon emissions has attracted huge attention from academic and industry communities for developing renewable energy sources and carbon capture techniques. Nonthermal equilibrium plasma catalysis has been proven to be a very promising way for CO2 conversion into high-value-added products; however, the synergistic catalytic mechanism between the plasma and various catalysts remains a challenge. In this work, we designed a reactor of atmospheric pressure glow discharge (APGD) plasma jet coupled with V2O5/TiO2 nanocomposite catalysts and studied the influence of V2O5 mass fraction, catalyst pretreatment, and reaction plasma parameters on the CO2 dissociation performance. Results showed that the designed reactor could introduce high-density plasma to the downstream area and maintain lower gas temperature, allowing the collaboration between APGD and the V2O5/TiO2 catalyst. The XRD analysis indicated that the solid solution phase TiVO4 could be formed in catalysts by V2O5 doping and reach a maximal content at a mass fraction of 30%, which determined the most excellent redox ability of the catalyst. The pretreatment of the as-prepared catalyst by Ar dielectric barrier discharge (DBD) plasma increased the oxygen vacancy density of the catalyst, thereby raising the conversion rate by 18.43%. Moreover, the transition regime between laminar and turbulent states was found to be the optimal configuration for CO2 dissociation. The reaction pathway was proposed for CO2 dissociation synergistically catalyzed by an APGD plasma jet and V2O5/TiO2. Ultimately, the maximum conversion of 14.88% and energy efficiency of 40.45% were simultaneously achieved, which were superior to the results of most atmospheric pressure plasmas. This work opens an avenue to develop plasma technology for sustainable CO2 utilization.
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ENERGY & FUELS
·
2023
·
IF 5.3
Xianhang Jin,Enze Ren,Min Zheng,Xiurong He,Yun Yang
A CO2 phase change absorbent (CPCA) is of interest because it has the potential to reduce energy consumption for CO2 capture. Controllable phase separation behavior was expected in the development and application of a CPCA. In this study, the effects of CO2 loading under different activators and physical solvents on the phase separation behavior of an activated methyldiethanolamine (MDEA)-based CPCA were investigated. By adjustment of the CO2 loading, controllable phase separation behavior was achieved and the absorbent comprising an activator with more −NH– groups and a physical solvent with low ET(30) was favored to exhibit phase separation. Of special interest was that, with the increasing of CO2 loading, phase behaviors, from the liquid phase to solid–liquid phase and then to the liquid phase, were observed for CPCA comprising MDEA/piperazine (PZ)/N-methyl-2-pyrrolidone (NMP), which was different from all of the other known CPCAs. The solid compound was identified as PZ carbamate by X-ray diffraction (XRD), Fourier transform infrared (FTIR), and elemental analysis, and the liquid-phase samples were detected by 13C nuclear magnetic resonance (NMR). The phase change mechanism of this special phenomenon was proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lulu Zhao,Huilin Hou,Lin Wang,Chris R. Bowen,Jinguo Wang,Ruifang Yan,Xiaoqiang Zhan,Hongli Yang,Man Yang,Weiyou Yang
Creating useful chemicals based on artificial CO 2 photoreduction is considered to be an attractive approach to address the environmental and energy crises. Currently, its selectivity with high conversion efficiency is still a grand challenge. Here, we report the refined substitution of Bi 3+ with Ag + in ultrathin Bi 2 WO 6 nanosheets through a liquid-phase cation exchange process, favoring a high selectivity towards the photocatalytic production of CO from CO 2 . The incorporation of Ag + could not only significantly promote the adsorption of both CO 2 and H 2 O molecules, but also facilitate the transfer of photogenerated carriers. The as-fabricated photocatalyst achieves a high CO generation rate of 116.96 μmol g −1 with a superb selectivity of 95.7 % after 6 h reaction without any sacrificial agent, approximate 4.2 times higher than that of pure Bi 2 WO 6 . The mechanism for photocatalytic CO 2 reduction is proposed, based on in-situ Fourier Transform Infrared spectrometry analyses and Density Functional Theory calculations.
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