ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Shuhui Wang,Jiawei Zhan,Kui Chen,Asad Ali,Linghui Zeng,He Zhao,Wanglai Hu,Lixin Zhu,Xiaoliang Xu
The visible-light-driven CO2 reduction efficiency is largely restrained by the negative photoabsorption and high recombination rate of electron–hole pairs. It is an effective method to increase the efficiency of CO2 photoreduction by doping alkali metal elements to engineer the electronic properties of the catalyst. Here, we report a new study on the potassium-doped g-C3N4 (K-CN) being used for CO2 reduction irradiated by visible light. DFT calculations and XPS tests show that the potassium doping is interlayer doping, changing the electronic structure of g-C3N4. The higher ID/IG value indicates more structural distortion and defects caused by K doping. K-CNs have enhanced visible-light absorption, and PL spectra demonstrate that the introduction of potassium advances the separation and transmission of photoexcited charge carriers, further confirmed by transient photocurrent response experiment. Under visible light, K-CN-7 achieved efficient CO2 reduction without any noble metal as a cocatalyst, with CO formation rates of 8.7 μmol g–1 h–1, which is 25 times that of ordinary g-C3N4. Our work further validates the importance of inhibiting e–/h+ recombination in improving solar energy conversion efficiency while also bringing hope for efficient solar fuel production using g-C3N4.
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STAR Protocols
·
2023
·
IF 0
Shuchao Jiang,Jikai Sun,Guoqing Ren,Weiqiao Deng
Summary CO 2 capture and utilization into liquid fuels and high-added-value chemicals has been regarded as an attractive strategy to mitigate excessive carbon emissions. Here, we present a protocol to capture and convert CO 2 into pure formic acid (HCOOH) solution and solid fertilizer (NH 4 H 2 PO 4 ). We describe steps for synthesis of an IRMOF3-derived carbon-supported PdAu heterogeneous catalyst (PdAu/CN-NH 2 ), which can efficiently catalyze (NH 4 ) 2 CO 3 -captured CO 2 into formate under ambient conditions. For complete details on the use and execution of this protocol, please refer to Jiang et al. (2023). 1
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PubMed
JOURNAL OF MOLECULAR LIQUIDS
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2018
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IF 4.513
Guang Zhao,Xuepeng Wu,Rizhong Luan,Shaikh Azizullah,Haiming Fan,Caili Dai
A novel CO 2 responsive anionic smart wormlike micelles (SWLMs) was constructed by simply mixing sodium oleate (NaOA) and the small organic counterion 2, 6, 10-trimethyl-2, 6, 10-triazaundecane (TMTAD) in a 3:1 M ratio without complex organic synthesis. After bubbling CO 2 , TMTAD and NaOA molecules in aqueous solution, a pseudo Gemini surfactant is formed in situ due to electrostatic interactions. This system shows two obvious performance transitions when CO 2 is continuously introduced, from a water-like solution to a viscoelastic fluid and then a milky solution. Such transitions reflect the continuous transformation of the self-assembled structure from spherical micelles to wormlike micelles and then vesicle or spherical micelles. Additionally, this system can exhibit two similar sequential transformations when the pH changes in the reverse process.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Zhiliang Wu,Wei Li,Linlin Hou,Qiuming Wei,Huixing Yang,Yangyang Jiang,Dingyuan Tang
Metal-organic framework (MOF) and covalent organic framework (COF) hybrid materials have drawn much research attention in the field of photocatalysis due to their complementary advantages, massive specific area, customizable structure and performance, and suitable band gap. Herein, the MOF@COF hybrid platform with a novel sunflower-like strong π-π bond stacking was formed by introducing the preformed synthetic COF into the MOF precursor solution and modulating its morphology by vacuum thermal-assisted growth. More importantly, the synthesized MOF on the COF hybrid platform with multiple active centers exhibits excellent catalytic activity in the sacrificial agent-free photocatalytic CO 2 reduction reaction under simulated sunlight. Additionally, the maximum CH 4 yieldrate of the synthesized PCN-222-Cu@TpPa-1 (1:2) reached 21.27 μmol g -1 h -1 , with an AQY (apparent quantum yield) about 10.46 % (in pure water system, λ = 550 nm) and a methane selectivity of about 27.25 %. The best performance of PCN-222-Cu@TpPa-1 is approximately 4.3 times higher than that of pure PCN-222-Cu and 100 times higher than that of the reported NH 2 -MIL-125(Ti) NMB. The selectivity of the products CO and CH 4 can be improved by adjusting the ratio of MOF and COF. Finally, the goal of providing an optimal photocatalytic platform for increased photocatalytic CO 2 reduction with highly effective morphology-tunable MOF@COF was expanded upon by a potential photocatalytic reaction mechanism, which was suggested based on the analysis of experimental results.
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Nature Communications
·
2025
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IF 15.7
Han Songyue,He Linhai,Chen Nan,Fan Dong,Tian Peng,Liu Zhongmin
Selective hydrogenation of CO 2 into high-value C 2+ oxygenates, such as acetic acid (AA), methyl acetate (MA), and ethanol, is highly attractive yet remains a significant challenge. This study demonstrates an innovative tandem catalysis system for converting CO 2 to AA and MA, employing GaZrO x and hydrophobically modified MOR-8-C1@PC (PTFE+CNTs) catalysts. The upstream GaZrO x drives CO 2 hydrogenation to produce an effluent gas with a controlled CO/(DME + CH 3 OH) ratio of approximately 4, facilitating the subsequent carbonylation reaction over the MOR-based catalyst. For the downstream catalyst, surface silanization of MOR zeolite combined with a hydrophobic promoter effectively prevents water (generated during CO₂ hydrogenation) from entering the zeolite channels and greatly enhances the carbonylation activity and catalyst stability. Results show that at a CO 2 conversion of 27%, the selectivity towards AA and MA in the organics reaches up to 78%, with no catalyst deactivation observed over 50 hours. This strategy offers an efficient approach for converting CO 2 into C 2+ oxygenates, with promising implications for sustainable chemical production.
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PubMed
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Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 17
·4369-4375
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IF 7.779
Xuyang Chen,Meiyu Cong,Ming Tang,Jinxuan Liu,Shaoyun Chen,Yan Gao
A bimetallic ZnCo-porphyrin metal–organic framework (ZnCo-BMOF) nanosheet was developed for efficient photoreduction of CO2 to CO. The ZnCo-BMOF nanosheet comprises photosensitizers (Zn porphyrin) and catalysts (Co porphyrin) providing a molecular platform to enable fast electron transfer from photosensitizers (PSs) to atomically dispersed catalytic Co sites. Under visible light illumination, the ZnCo-BMOF nanosheet can efficiently reduce CO2 to CO with a yield of 778 μmol g−1 in 6 h, which is 2.8-fold higher than those of its counterparts (Zn-MOF/Co-MOF = physically mixed Zn-MOF and Co-MOF), owing to the improvement of charge transfer capacity and longer lifetime of the photogenerated electron–hole pairs. Density functional theory calculation results reveal that atomically dispersed cobalt sites serve as efficient active sites, which favors accepting electrons from the Zn porphyrin.
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Catalysis Science & Technology
·
2016
·Vol. 6
·期 22
·7967-7975
·
IF 5.287
Jie Zhao,Yun Wang,Yingxuan Li,Xiu Yue,Chuanyi Wang
CeO2 is a basic promoter for CO2 photoreduction with H2O over TiO2-based catalysts, but there is still a lack of insight into the interaction of CeO2 with different TiO2 polymorphs and its effect on CO2 photoreduction. In this study, pure anatase, brookite, and rutile TiO2 and their respective hybrids with CeO2 were prepared, and their structural properties, optical properties, interfacial interaction and activity for CO2 photoreduction were systematically studied. The addition of CeO2 improved the activity for CO2 photoreduction under simulated sunlight irradiation, but the improvement depends on the phases of the TiO2. X-ray diffraction, macro-Raman spectroscopic and electron paramagnetic resonance measurements confirm the presence of Ti defects at the CeO2–rutile interfaces, implying a relatively strong interaction between CeO2 and rutile, which is beneficial for the interfacial separation of photogenerated charge carriers. As a result, CeO2/rutile shows the best enhancement of CO2 photoreduction among the studied CeO2/TiO2 systems. Moreover, different paramagnetic species were detected in the three TiO2 polymorphs. The O− radical anion in the anatase lattice could be oxidized to produce Ti3+ under UV-light irradiation, whereas the O2− radical anion on the surface of brookite TiO2 might retard CO production.
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Nano Energy
·
2019
·
IF 15.548
Xiaoli Jin,Chade Lv,Xin Zhou,Haiquan Xie,Shanfu Sun,Yue Liu,Qingqiang Meng,Gang Chen
The insufficient separation of photogenerated charge carriers and faint CO 2 capture remains the major obstacles for photocatalytic conversion of CO 2 into solar fuel. Rational design of semiconductor photocatalysts with unique structures may be promising to break this bottleneck. Herein, bismuth rich Bi 4 O 5 B 2 hollow microspheres are designed as a robust photocatalyst for efficient CO 2 reduction. Thanks to the bismuth rich strategy, the highly dispersed band structure and the elevated conduction band (CB) potential facilitate the charge transfer and photoreduction ability. Meanwhile, hollow structure provides the large specific area and creates a resonance in its interior to enhance the CO 2 adsorption and activation. Benefiting from the collaborative promotion effect, the local charge arrangement and electronic structure are tuned so as to an exceptional efficiency of photocatalytic CO 2 conversion into CO (3.16 μmol g −1 h −1 ) and CH 4 (0.5 μmol g −1 h −1 ) is attained over hollow Bi 4 O 5 Br 2 , which is superior to that of solid Bi 4 O 5 Br 2 and BiOBr, as well as other reported Bi-based photocatalysts. This work paves new opportunities for exploring high-efficiency CO 2 photoreduction catalysts.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yang Zhang,Yue Zhang,Yilei Yan,Yuchao Ma,Kaihua Li,Shuo Yang,Long Jiao,Shaofei Wang,Bowen Cheng,Leixin Yang
Covalent organic frameworks (COFs) are promising membrane materials for gas separation due to their periodic pore structure and chemical tailorability. However, the COF membranes usually show oversized pores and a single separation mechanism, which limits their gas separation applications. In this work, we fabricate highly ordered covalent organic framework (COF) membranes through interfacial polymerization, guided by a nucleation–epitaxial growth mechanism that ensures dense and defect-free layers. By regulating monomer hydroxyl content and spatial distribution, we achieve tailored pore architectures and interlayer stacking. Furthermore, a microenvironment engineering strategy is implemented via post-modification with boric acid and piperazine, which fine-tunes the pore size and introduces CO 2 -philic sites, enabling a synergistic combination of diffusion selective and facilitated transport. The optimized membrane exhibits an evident pore contraction, with the average pore diameter decreasing from 2.04 nm to 1.06 nm, confirming the effective tuning of the internal channels. As a result, it delivers a high CO 2 permeance of 2149 GPU and a CO 2 /N 2 selectivity of 14.3. This microenvironment regulation approach reveals critical structure–property relationships and provides valuable guidance for the separation of small molecule mixtures by large-pore membrane materials.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Shuangjiang Li,Yi Liu,Lan Shi,Tianding Hu,Mengrui Li,Churu Zhang,Shaoyun Shan,Yunfei Zhi
A Salen-functionalized ionic polymer (Zn-Salen-IP) was synthesized through a metal-assisted method. The structure and microstructure were characterized by using different characterization methods. Subsequently, the cycloaddition of CO 2 with epoxide was used to investigate the catalytic activity of Zn-Salen-IP. The relationship between the types of ions within Zn-Salen-IP and its catalytic performance was thoroughly explored. Single-factor investigations were used to determine the optimal reaction conditions for catalytic CO 2 cycloaddition used Zn-Salen-IP. The universality and recyclability of Zn-Salen-IP were systematically studied under the optimized conditions. Finally, Density functional theory calculations were employed to research the mechanism and pathway of the CO 2 cycloaddition reaction catalyzed by Zn-Salen-IP with dual functional active sites. This provided a deep understanding for the rate-determining step and the influence of the nucleophilicity of the halogen anion in cycloaddition reaction of CO 2 and epoxide.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Shuai Yan,Yuting Wang,Guangyao Chen,Wanli Ma,Yingquan Chen,Xianhua Wang,Kuo Zeng,Yonggang Yao,Hongqi Sun,Haiping Yang,Hanping Chen
Transition metals doping for Fe-based catalysts has been demonstrated in promoting the activity and regulating the selectivity in both reverse water gas shift reaction and Fischer-Tropsch synthesis. However, there are few studies that concern their catalytic performances tailored by these promoters under photothermal conditions. In this study, a series of typical MFeOx (M = Mn, Co, Cu, Zn) catalysts were synthesized with a facile co-precipitation method and their photothermal CO2 hydrogenation properties were evaluated. The results showed that the doping of Co, Cu, and Zn enhanced the activity and regulated the selectivity of Fe-based catalysts, e.g., CoFe achieving a C2+ yield of 1.73 mmol·h-1·g-1 while ZnFe almost doubling the CO2 conversion under irradiations. Mechanistic studies suggest that Co and Cu facilitated the reduction of Fe species, resulting in favorable CO2 and H2 activation. At last, a light-induced direct CO2 dissociation pathway was proposed with in situ EPR and DRIFTS characterization and analysis of the undoped Fe and ZnFe catalyst. This study provides a novel perspective on transition metal promoters for photothermal CO2 hydrogenation over Fe-based catalysts.
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ACS Nano
·
2024
·
IF 15.8
Xue Tian,Huan Liu,Bin Cao,Peng Zhang,Yanze Li,Yanchao Ou,Haonan Cui,Mengyao Xu,Bin Xu
MXenes are promising cathodes for Li–CO2 batteries owing to their high electrical conductivity and efficient CO2 activation function. However, the effects of adsorption and electronic structures of MXene on the full life cycle of Li–CO2 batteries have been rarely investigated. Here, we employ a coregulation approach to enhance the adsorption–decomposition of lithium carbonate (Li2CO3) by introducing Zn and Cl surface groups onto the Ti3C2 MXene (Zn–Ti3C2Cl2) catalyst. The incorporation of Cl surface groups enhances Li2CO3 adsorption on the MXene catalyst surface, resulting in the formation of small-sized and uniform Li2CO3. Additionally, the introduction of Zn shifts the d-band centers of titanium and promotes CO2 evolution reaction (CO2ER) activity, thereby facilitating the decomposition of discharge products. As a result, the Li–CO2 battery based on the Zn–Ti3C2Cl2 catalyst exhibits an ultralow overpotential (0.72 V) at 200 mA g–1 and stable cycling for up to 1500 h. This work validates the efficacy of promoting reversibility in Li–CO2 batteries by adjusting the adsorption-decomposition process.
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