DALTON TRANSACTIONS
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2024
·Vol. 53
·期 23
·9724-9731
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IF 3.5
Ying Peng,Shuo Chen,Zhengli Hu,Mengqi Yin,Lishun Pei,Qiaohua Wei,Zailai Xie
Developing novel electrocatalysts for achieving high selectivity and faradaic efficiency in the carbon dioxide reduction reaction (CO2RR) poses a major challenge. In this study, a catalyst featuring a nitrogen-doped carbon shell-coated Ni nanoparticle structure is designed for efficient carbon dioxide (CO2) electroreduction to carbon monoxide (CO). The optimal Ni@NC-1000 catalyst exhibits remarkable CO faradaic efficiency (FECO) values exceeding 90% across a broad potential range of −0.55 to −0.9 V (vs. RHE), and attains the maximum FECO of 95.6% at −0.75 V (vs. RHE) in 0.5 M NaHCO3. This catalyst exhibits sustained carbon dioxide electroreduction activity with negligible decay after continuous electrolysis for 20 h. More encouragingly, a substantial current density of 200.3 mA cm−2 is achieved in a flow cell at −0.9 V (vs. RHE), reaching an industrial-level current density. In situ Fourier transform infrared spectroscopy and theoretical calculations demonstrate that its excellent catalytic performance is attributed to highly active pyrrolic nitrogen sites, promoting CO2 activation and significantly reducing the energy barrier for generating *COOH. To a considerable extent, this work presents an effective strategy for developing high-efficiency catalysts for electrochemical CO2 reduction across a wide potential window.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yunpeng Wang,Tao Liu,Chun Cheng,Yachen Xie,Cheng Lan,Wenchuan Jiang,Zhiyu Zhao,Shuo Zhai,Yiri Li,Yifan Wu,Heping Xie
CO 2 batteries offer a promising avenue for mitigating CO 2 emissions and conversion, but encounter challenges such as high costs, dendrite, corrosion, flooding and slow kinetics stemming from the use of metal electrodes. CO 2 mineralization is thermodynamically favorable (ΔG CO2 ), presenting an opportunity for processing solid waste and reducing CO 2 emissions while potentially producing energy. However, the lack of direct electron transfer in the CO 2 mineralization reaction hinders the direct generation of electrical energy. Here, we propose an organic CO 2 mineralization battery (OCMB) without using metal, which efficiently harnesses CO 2 to mineralize solid waste carbide slag, maximizing the recovery of mineralization reaction energy to generate electricity and produce carbonate products, without requiring renewable electricity charging. We employ a high-solubility, stable under strong alkaline conditions, and fast kinetics organic phenazine derivative—DSPZ as the electron and proton carrier, which facilitates the conversion of ΔpH between electrodes by interacting with alkaline wastes and CO 2 into electricity. Simultaneously, the OCMB undergoes regeneration cycles through mineralization reactions. The theoretical model predicted the open circuit voltage (OCV) and discharge behavior of OCMB, offering insights for improved battery engineering. We demonstrate an impressive peak power density exceeding 227.5 W/m 2 for the OCMB, with an estimated electricity production of ∼ 178.03 kWh per ton of CO 2 mineralization. This research underscores the potential integration of OCMBs into CO 2 energy systems, waste treatment processes, and chemical production, offering both economic and environmental benefits.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-15
·
IF 14.7
Yao Zhibo,Cheng Hao,Xu Yifei,Zhan Xinyu,Hong Song,Tan Xinyi,Wu Tai-Sing,Xiong Pei,Soo Yun-Liang,Li Molly Meng-Jung,Hao Leiduan,Xu Liang,Robertson Alex W.,Xu Bingjun,Yang Ming,Sun Zhenyu
The electrocatalytic reduction of CO 2 to CO is slowed by the energy cost of the hydrogenation step that yields adsorbed *COOH intermediate. Here, we report a hydrogen radical (H•)-transfer mechanism that aids this hydrogenation step, enabled by constructing Ni-partnered hetero-diatomic pairs, and thereby greatly enhancing CO 2 -to-CO conversion kinetics. The partner metal to the Ni (denoted as M) catalyzes the Volmer step of the water/proton reduction to generate adsorbed *H, turning to H•, which reduces CO 2 to carboxyl radicals (•COOH). The Ni partner then subsequently adsorbs the •COOH in an exothermic reaction, negating the usual high energy-penalty for the electrochemical hydrogenation of CO 2 . Tuning the H adsorption strength of the M site (with Cd, Pt, or Pd) allows for the optimization of H• formation, culminating in a markedly improved CO 2 reduction rate toward CO production, offering 97.1% faradaic efficiency (FE) in aqueous electrolyte and up to 100.0% FE in an ionic liquid solution.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shujie Liang,Jiaxin Lv,Yishun Wang,Hong Deng
The development of efficient and stable single-atom catalysts (SACs) for CO 2 photoreduction is a persistent challenge. This study reports the successful preparation of SACs by incorporating isolated Ni atoms into carbon nanorods through a low-temperature calcination process using nickel bis(dimethylglyoximate) complexes. These Ni atoms, maintaining their original coordination environments, can facilitate charge separation, and enhance CO 2 adsorption and activation. The optimized catalyst exhibits a CO formation yield of 24.4 µmol with ∼96 % selectivity in high-purity CO 2 , outperforming both the precursor and pure carbon. Additionally, the Ni SACs showed strong catalytic selectivity in diluted CO 2 conditions, with selectivity rates of 82.57 %, 80.35 %, and 61 % at 0.1, 0.05, and 0.01 atm, respectively. This work provides critical insights for designing efficient visible light-responsive CO 2 photoreduction catalysts at the atomic level.
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ACS Materials Letters
·
2024
·
IF 9.6
Cun Chen,Honggang Huang,Yao Chen,Zhe Zhang,Hui Fu,Hanjun Li,Wei-Hsiang Huang,Feili Lai,Nan Zhang,Tianxi Liu
Interface engineering has been widely explored due to its potential for regulating the intermediate adsorption, controlling mass/electron transfer, and preventing severe aggregation of catalysts. Hence, we have synthesized a series of Cu–In metallic aerogels (MAs) with a controlled ratio of Cu/Cu2In interfaces as efficient catalysts for electrochemical carbon dioxide reduction reaction (CO2RR). As a result, Cu–In MAs with the highest Cu/Cu2In interfaces abundance (Cu2In MAs) achieve the high Faradaic efficiency of CO up to 94.5% at −0.6 V vs reversible hydrogen electrode (RHE), outperforming Cu1In MAs, Cu3In MAs, Cu4In MAs, and Cu MAs. Furthermore, Cu2In MAs with the highest Cu/Cu2In interface abundance also exhibit excellent stability after continuous electrolysis for 10 h. Mechanism research indicates that the rich Cu/Cu2In interfaces in Cu2In MAs allow for moderate adsorption of CO2 and accelerate electronic transmission, which greatly reduce the energy barrier of the potential-limiting step, thus improving the CO2RR performance. This study indicates that interface engineering plays an important role in improving the CO2RR performance, providing a new strategy for preparing efficient CO2RR catalysts.
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Biomass Conversion and Biorefinery
·
2025
·
IF 4.1
Zhao Xiaoben,He Tao,Wang Shuainan,He Song
In this research, nitrogen-doped activated carbons (NACs) featuring a high specific surface area (3396 m 2 /g) and a certain amount of nitrogen doping (0.79–1.69%) were prepared by a combination of chemical activation and self-activation methods, and their CO 2 adsorption characteristics were comprehensively assessed. The experimental results showed that nitrogen doping not only significantly enhanced the specific surface area of the materials, but also significantly enhanced the CO 2 adsorption. The CO 2 adsorption capacity of the optimal sample, CMAC-0.5–3-700, reached 4.11 mmol/g and 2.32 mmol/g at 0 °C and 25 °C, respectively. In addition, the selectivity of NACs for CO 2 /N 2 was significantly improved, with a selectivity factor of up to 50.16, and the competitive adsorption experiments also demonstrated that NACs could still effectively adsorb CO 2 under the condition of CO 2 /N 2 = 15/85. Density-functional theory (DFT) calculations further revealed the interaction mechanism between NACs and CO 2 molecules, the enhanced CO 2 selectivity is attributed to electrostatic and π-electron interactions between nitrogen atoms and CO 2 . The findings indicate the significant potential of nitrogen-doped activated carbons (NACs) with high specific surface area and substantial nitrogen doping for post-combustion CO 2 capture.
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Manman Zhang,Liu Chen,Kaifang Wang,Ruitao Lin,Zeshen Xiao,Raphael Semiat,Xuezhong He
The development of materials has given rise to the study and design of poly(ionic liquid)s (PILs) for making CO2-selective membranes. The huge design space for the chemical structures of PILs provides great opportunities to further investigate the factors underlying gas permeability and selectivity. Herein, copolymerizing imidazolium-based ionic liquid (IL) monomers with two functionalized monomers of acrylamide (AM) and butyl acrylate (BA) based on free radical polymerization was conducted, and the effect of the chemical structures for PIL-based copolymers on their performances of derived membranes for CO2/N2 separation was evaluated. Nuclear magnetic resonance (NMR) and Fourier transform infrared (FTIR) spectroscopy analysis confirmed the successful synthesis of copoly(ionic liquids) (co-PILs) with the designed chemical structures. The co-PIL-based composite membranes were fabricated by coating the copolymer solutions on the surface of a commercial polysulfone (PSF) membrane. It was found that the best composite membranes present significantly enhanced CO2 permeance (76 GPU) and CO2/N2 selectivity (53) by 262% and 61% compared to pure PSF membranes. The proposed coating method using co-PILs provides a facile solution to improve the CO2 separation membrane performance. Therefore, molecular engineering of the chemical structures for poly(ionic liquids) opens a venue to develop high-performance co-PIL-based membranes for potential CO2 capture from flue gases.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Qi Liu,Tong Luo,Yiyan Yin,Yan Ouyang,Min Xiao,Hongxia Gao,Teerawat Sema,Zhiwu Liang
Amine degradation is one of the key issues that hampers the implementation of amine-based post combustion carbon capture technology. In this work, the oxidative degradation of fourteen structurally varied amines were experimentally studied by measuring the amine loss, alkalinity change, ammonia yield, and degradation product. There is a linear relationship between amine loss against alkalinity change and ammonia yield, indicating that the degradation product either loss reactivity for CO 2 absorption or emit out as the small molecule. The results have shown that amine stability generally increased with amine order and stronger steric hindrance effect. Most primary and secondary amines showed more than 40 % amine loss after 336 h degradation experiment, while most of tertiary amines showed less than 10 % amine loss. This may be due to the exposed amine groups of primary and secondary amines. The oxidative degradation mechanism was studied based on density functional theory (DFT) calculations.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
·
IF 3.141
Pengcheng Zhu,Zhixin Liu,Jun Nie,Yong He
CO2-responsive and photopolymerizable prepolymers are designed and synthesized. Their good photopolymerization kinetics and reversible CO2 and N2 responses to a bulk state and in a solution are reported. Stepwise modulation is verified in template imprinting. Results reveal that stable and high-resolution patterns can be produced by imprinting liquid prepolymers in CO2 atmosphere, erased by warm heating, or retained permanently by chemical cross-linking through photopolymerization with the aid of a photoinitiator. By contrast, only blurry patterns are obtained in air.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Changwei Chen,Yanke Yu,Chi He,Li Wang,Huang Huang,Reem Albilali,Jie Cheng,Zhengping Hao
Four kinds of carbon-based adsorbents (micro-mesoporous hybrid carbon nanosphere and N-doped hollow carbon sphere with single-, double- or ruga-shell morphology) with different structural and textural properties were prepared and systematically studied in CO 2 capture. All synthesized samples possess high specific surface area (828–910 m 2 g −1 ), large pore volume (0.71–1.81 cm 3 g −1 ), and different micropore contents varied from 2.1% to 46.4%. Amongst, the ordered micro-mesoporous carbon nanosphere (OM-CNS) exhibits the best adsorption performance with CO 2 uptake as high as 3.01 mmol g −1 under conditions of 298 K and 1.0 bar, better than most of the reported CO 2 adsorbents. The excellent CO 2 adsorption capacity of OM-CNS can be reasonably attributed to the synergistic effect of ordered mesopore channels and abundant structural micropores which are beneficial for the diffusion and trapping of CO 2 adsorbate. Moreover, the OM-CNS shows excellent CO 2 trapping selectivity and superior stability and recyclability, which endow the OM-CNS as a promising and environmental-friendly adsorbent for CO 2 capture and separation under practical conditions.
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Catalysts
·
2018
·Vol. 8
·期 2
·78
·
IF 3.465
Yebin Guan,Ming Xia,Alessandro Marchetti,Xiaohong Wang,Weicheng Cao,Hanxi Guan,Xueqian Kong
Photocatalytic reduction with sunlight is an economical and promising advanced approach for reducing the excessive emissions of CO2from the combustion of fossil fuels. Aimed at practical applications, a type of inexpensive colored anatase material was used to evaluate CO2photoreduction performance on a platform with a continuous flow of gas mixtures (10 vol % CO2, 90% N2), which resembles realistic flue gas conditions. The results showed an enhanced photocatalytic activity compared with standard P25 and significant improvement over pristine anatase. Based on a series of characterization techniques, we propose that the oxygen vacancies and surface hydroxyl groups on colored anatase can reduce the bandgap and assist the binding of CO2molecules. Our results showed that photoreduction of CO2is feasible under practical conditions, and the efficiency could be improved through modification of catalysts.Keywords:photocatalytic reduction;TiO2;anatase;CO2;flue gas
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Hao Zheng,Guoliang Guo,Xiaoqiang Pei,Pengke Huang,Xiaoling Liu,Wenge Zheng
Elastomer foams with customized multimodal cellular structures have great application requirements in advanced fields, but a simple and practical way to realize it needs to be further studied. Herein, a strategy of presetting cells into elastomers before supercritical CO2 foaming was introduced to customize the cellular structures. Typically, taking olefin block copolymers (OBC, a thermoplastic elastomer with crystalline hard segments and rubbery soft segments) foams as an example, bimodal, sandwich, and gradient multimodal cellular structures were successfully prepared. The interaction between preset cells and newly nucleated cells during foaming had been systematically studied by controlling the morphology of preset cells and foaming conditions. It was found that the configuration of preset cells and the nucleation rate of small cells in OBC foams had a significant impact on their cellular structures. Specifically, the bimodal cellular structures can improve the expansion ratio and elasticity of OBC foams, and their rebounding ability could be improved by 14%, while their energy loss coefficient would be decreased by 17% (compared to homogeneous ones in this study). Furthermore, the feasibilities of this strategy in other elastomer foams (like POE, EPDM, and EVA foams) with bimodal cellular structures were also verified, which was expected to promote the development of high-performance elastomer foams.
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