ACS Applied Materials & Interfaces
·
2022
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IF 10.383
Xiangfu Meng,Guoxing Pan,Hongji Liu,Yong Qian,Xingyu Wang,Changlai Wang,Lin Hu,Hui Wang,Qianwang Chen
The electroreduction of carbon dioxide (CO2) to a liquid product is a viable method for establishing an artificial carbon cycle. Unfortunately, most electrocatalysts’ low efficiency and instability prevent them from being used in practical applications. In the current study, we developed ultrasmall Cu nanocrystals embedded in nitrogen-doped carbon nanosheets (Cu/NC-NSs) for selective CO2 electroreduction by adjusting the potential. Cu/NC-NSs had 43.7 and 63.5% Faradaic efficiencies for the synthesis of ethanol and formate with applied potentials of −0.37 and −0.77 V vs reversible hydrogen electrode (RHE) using a flow cell architecture, respectively. Moreover, these Cu/NC-NSs show a steady catalytic performance up to 16 h. Density functional theory (DFT) calculations were performed to investigate the reaction mechanism. Furthermore, the synergistic effect formed by nitrogen-doped carbon and highly dispersed copper atoms led to their excellent performance in CO2 electroreduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yang Hong,Yan Zhou,Jiaqi Chen,linqian Qin,Yongqi Li,Yang Li,Hongyan Jiang,Huiyang Zhao,Jinzhu Wu,Xiaohong Wu
Advances in carbon capture and storage (CCS) technologies are critical for mitigating global climate change due to their low cost and operational simplicity. Although zeolites hold promise for carbon capture, the development of advanced zeolite materials with optimized CO 2 separation efficiency and diffusivity remains challenging. In this study, we present a quantum dot-regulated growth strategy, in which silicon quantum dots (SiQDs) act as heterogeneous seeds to not only initiate the growth of nanoscale zeolite units but also guide their assembly. The resulting 13X-SiQDs exhibit a distinct micrometer-scale hollow sphere structure composed of nanoscale zeolite units, which provide additional adsorption sites and mesopores, significantly enhancing adsorption and diffusion. The amino groups on the surface of the SiQDs further enable chemical adsorption with CO 2 , strengthening the binding force. The synergistic combination of thermodynamic and kinetic advantages enables 13X-SiQDs to achieve substantial improvements in CO 2 adsorption capacity (132.20 cm 3 ·g −1 ), CO 2 /N 2 selectivity (561), and diffusion rate. This quantum dot-regulated synthesis strategy offers a promising approach for designing advanced adsorption materials with high performance, extending their potential applications beyond carbon capture.
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RARE METALS
·
2025
·
IF 11
Zheng Zi-Chen,Liu Ke-Wei,Zhou Yi-Wen,Zhang Zi-Cong,Qin Yong-Bin,Luo Yi-Fan,Xu Kai-Chun,Guo Liang-Chao,Debliquy Marc,Bittencourt Carla,Zhang Chao
Bismuth-doped antimony tungstate (Bi-doped Sb 2 WO 6 ) microspheres were synthesized via a novel hydrothermal synthesis approach. These microspheres were then used as active layers in gas sensors for the detection of carbon dioxide (CO 2 ), a significant greenhouse gas and a critical parameter for evaluating air quality. The incorporation of bismuth significantly enhances the gas-sensing performance of the Sb 2 WO 6 microspheres, with the 4% Bi-doped sensing active layer achieving a remarkable response value of 15 when exposed to 200 ppm of CO 2 , outperforming the undoped Sb 2 WO 6 . Furthermore, the selectivity of the 4%Bi-Sb 2 WO 6 sensor toward CO 2 gas was enhanced relative to the Sb 2 WO 6 sensor. The fundamental mechanisms of gas sensing and the factors contributing to the improved CO 2 response of 4%Bi-Sb 2 WO 6 microspheres were investigated using density functional theory. Bi-doped Sb 2 WO 6 materials exhibit significant advantages in gas-sensing applications, including improved conductivity, enhanced gas adsorption capacity, increased reaction rates, good chemical stability, excellent selectivity, and the ability to adjust electron density. These characteristics enable Bi-doped Sb 2 WO 6 to demonstrate higher sensitivity and rapid response capabilities in gas sensors, making it suitable for practical applications. Graphical abstract
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Jie Chu,Jialin Guo,Yafei Guo,Benshuai Guo,Pu Huang,Zhouzhou Zhang,Chuanwen Zhao
Integrating CO 2 capture and utilization (ICCU) in the production of syngas for the C1 chemical industry through ICCU-RWGS (reverse water–gas shift reaction) is a vital strategy for achieving carbon reduction, and designing highly active dual-functional materials (DFMs) capable of CO 2 adsorption and in-situ conversion is crucial. Alkaline lithium ceramics with high availability, featuring high CO 2 capture and catalytic performance, are promising DFMs candidates for ICCU-RWGS. Herein, lithium ceramics of Li 5 FeO 4, Li 6 CoO 4 and Li 6 ZnO 4 were prepared via solid state synthesis as potential DFMs for ICCU-RWGS applications, and structure-property-activity relationships of the lithium ceramics DFMs in ICCU were discussed. The Li-Zn sample with high surface basicity and high density and uniform dispersion of active sites demonstrated a high CO 2 uptake (7.71 mmol CO 2 /g), CO yield (6.52 mmol CO/g), CO 2 conversion (84.9 %) and CO selectivity (∼100 %) as well as moderate CO 2 adsorption and hydrogenation kinetics at 650 °C, 10 %CO 2 and 40 %H 2 , making it a promising candidate for ICCU-RWGS. However, the Li-Zn DFMs exhibited poor cyclic ICCU-RWGS working stability due to lithium sublimation and crystal sintering at high temperatures, which deserves more future efforts to solve the dilemma. Our findings provide valuable insights into designing cost-effective DFMs for ICCU applications.
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Membranes
·
2025
·Vol. 15
·期 1
·26
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IF 3.6
Rujing Hou,Junwei Xie,Yawei Gu,Lei Wang,Yichang Pan
Membrane technology is a promising methodology for carbon dioxide separation due to its benefit of a small carbon footprint. However, the trade-off relationship between gas permeability and selectivity is one obstacle to limiting its application. Herein, branched polyethyleneimine (BPEI) containing a rich amino group was successfully grafted on the surface of the metal–organic framework (MOF) of AIFFIVE-1-Ni (KAUST-8) through coordination between N in BPEI and open metal sites in the MOF and with the resultant maintained BET surface area and pore volume. Both the strengthened CO 2 solubility coefficients coming from the additional CO 2 adsorption sites of amino groups in BPEI and the reinforced CO 2 diffusivity coefficients originating from the fast transport channels created by KAUST-8 led to the promising CO 2 separation performance for KAUST-8@BPEI/Pebax-1074 MMM. With 5 wt.% KAUST-8@BPEI loading, the MMM showed the CO 2 permeability of 156.5 Barrer and CO 2 /N 2 selectivity of 16.1, while the KAUST-8-incorporated MMM (5 wt.% loading) only exhibited the CO 2 permeability of 86.9 Barrer and CO 2 /N 2 selectivity of 13.0. Such enhancement is superior to most of the reported Pebax-1074-based MMMs for CO 2 separation indicating a wide application for the coordination method for MOF fillers with open metal sites.
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Xiangzhu Ye,Jiawei Ruan,Lifang Chen,Zhiwen Qi
The integration of chemical absorption of CO 2 and in situ transformation to highly valuable chemicals is a promising process as an alternative toward fossil fuels . Here, three imidazolium ionic liquids (ILs), 1-butyl-3-methylimidazolium acetate, 1-butyl-3-methylimidazolium 1,2,4-triazole ([Bmim][Tz]), and 1-butyl-2,3-dimethylimidazolium 1,2,4-triazole were synthesized to absorb and activate CO 2 by the formation of CO 2 -adducts, which can be in situ converted into dialkyl carbonates with alcohols (ROH, R = CH 3 , C 2 H 5 , and C 4 H 9 ) in solvent diiodomethane under ambient temperature and pressure. The results show [Bmim][Tz] exhibits the best CO 2 absorption capacity and dimethyl carbonates (DMC) yield, where CO 2 capacity is up to 0.216 g CO2 /g IL and DMC yield (based on methanol) is as high as 20.2 %. The structures of imidazolium ILs have significant effects on the absorption of CO 2 and subsequent transformation process. Fourier transform infrared and carbon nuclear magnetic resonance spectroscopies demonstrate ILs structures influence binding sites for CO 2 absorption, which can combine with CO 2 to form CO 2 -adducts, zwitterion [Bmim-CO 2 ], and [Tz-CO 2 ] − . Furthermore, density functional theory calculations verify the structure effects (binding sites and steric hindrance) of ILs on the activation of CO 2 and methanol, through the elongated C O bond lengths of CO 2 -adducts and O-H bond lengths of methanol in IL-methanol complexes, respectively, leading to different DMC yields. The integrated process is promising for the energy-efficient capture and utilization of CO 2 under ambient conditions.
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Advanced Sustainable Systems
·
2025
·
IF 6.1
Qin Peng,Zhenxing Shen,Xinyu Mo,Tian Chang,Bo Song,Hao Fan,Zhenchuan Niu
The incorporation of functionalized secondary metal nodes into bimetallic metal–organic frameworks (MOFs) enhances their performance and application potential. This study investigates Cu/Zn-MOF-74 catalysts with varying metal ratios for carbon dioxide (CO₂)-epoxide cycloaddition. Compared to monometallic Cu-MOF-74 and Zn-MOF-74, the bimetallic system shows superior catalytic activity for epoxides conversion. Vim─COOH@Cu/Zn-MOF-74 is developed by introducing hydrogen bond donors (HBD) and nitrogen-containing linkers. The optimal Vim─COOH@Cu₀.₆₇Zn₀.₃₃-MOF-74 demonstrates outstanding performance in CO₂-epichlorohydrin cycloaddition, achieving 96.4% conversion and 98.5% selectivity under mild conditions (80 °C, 1.0 MPa, 24 h) without co-catalysts, while maintaining excellent recyclability. Using a one-pot synthesis, bimetallic MOFs with controlled Cu/Zn ratios are prepared. The framework is further modified by incorporating 1,4-butanediyl-3,3′-bis-1-vinylimidazolium bromide and HBD-functionalized imidazole bromide monomers. The resulting composites achieve over 80% conversion under solvent-free, co-catalyst-free conditions due to synergistic effects between Lewis acid sites, carboxyl groups, and nucleophilic Br⁻ ions. This work presents an effective strategy for developing efficient MOF catalysts for CO₂ conversion. The Vim─COOH@Cu/Zn-MOF-74 system demonstrates significant potential for sustainable CO₂ utilization in cyclic carbonate synthesis, combining high activity, selectivity, and stability under environmentally friendly reaction conditions.
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Molecular Catalysis
·
2025
·
IF 4.9
Xiaohong Guo,Liqiang Deng,Xiaoyue Wang,Yongjie Zhao,Zhifan Cao,Pengwei Li,Congming Li
A pivotal aspect in advancing ZrZnO x catalysts for CO 2 hydrogenation lies in the modulation of Zr-O-Zn active sites, with ZnO facets emerging as potential modulators of site activity. Whereas the beneficial influence of non-polar ZnO facets on ZrZnO x catalysts has been scarcely documented. Our investigation reveals that ZrZnO x catalysts exposed non-polar ZnO facets (ZrZnO-n) exhibit superior methanol selectivity (74 %) compared to those with randomly exposed ZnO facets (ZrZnO-r, 35 %). Characterization results demonstrate that it is ascribed to the formation of highly active Zr-O-Zn (2−δ)+ sites on ZrZnO-n, which facilitate H 2 adsorption and dissociation. In situ spectroscopic studies and DFT calculations further substantiate this finding, demonstrating enhanced intermediates formation and more efficient hydrogenation processes. This research underscores the significance of ZnO facet engineering in the purposeful creation of efficient ZrZnO x catalysts for CO 2 hydrogenation.
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Molecular Catalysis
·
2025
·
IF 4.9
Binxin Lv,Jiayue Yu,Fengchen Zhou,Zizi Wang,Junjun Zhang,Yifan Zhang,Yang Wu,Yong Wang,Wen Luo
Urea electrosynthesis plays a vital role in the nitrogen cycle, promoting carbon neutrality while also being energy-efficient. However, the complexities involved in the simultaneous of carbon and nitrogen-containing species significantly hinder the selectivity and yield of urea. In this study, we report a CuZn bimetallic catalyst that is capable of converting CO 2 and NO 3 ⁻ into urea, with a maximum Faraday efficiency of 40% at -0.6 V vs. RHE, alongside an impressive urea yield rate of 304.8 mmol h ⁻¹ g cat ⁻¹ at -0.9 V vs. RHE, surpassing the performance of both monometallic Cu and Zn catalysts. In situ spectroscopic analysis demonstrates that the Cu sites within CuZn facilitates the adsorption and activation of CO 2 and NO 3 ⁻ , while Zn sites additionally facilitate CO 2 adsorption and reduces the adsorption strength of *CO and *NH 2 on the catalyst surface, collectively promoting the formation of *CONH 2 as a key intermediate in urea synthesis. This study highlights the unique role of zinc in urea synthesis, offers new insights into optimizing the performance of copper-zinc catalysts, and serves as a valuable reference for future research on the role of zinc in urea synthesis.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
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IF 8.4
Zhicong Liang,Jiali Tang,Dario R. Dekel,Xuezhong He
Membrane separation is in the spotlight as one of the most cost-effective technologies without chemicals for carbon capture. This work aims to fabricate thin film composite (TFC) membranes for boosting CO 2 separation. Commercial polysulfone (PSf) flat sheet membranes pre-treated with ethanol solutions were used as support materials by coating with amino-functionalized cross-linked polydimethylsiloxane (PDMS) interlayer. It is worth noting that the developed amino-functionalized PDMS interlayer based on a novel wet-coating method to avoid the penetration of coating solution, which provides better compatibility with the coated polyamide selective layer and also the facilitated transport for CO 2 permeation. A thin CO 2 -selective layer was obtained by interfacial polymerization (IP) between trimesoyl chloride (TMC) in the organic phase and diethylene glycol bis(3-aminopropyl) ether (DGBAmE or EO3) in the aqueous phase to enhance the CO 2 /N 2 selectivity. Both the IP process and the membrane preparation parameters such as heat-treatment temperature, and monomer concentration were systematically optimized. It was found that the best membrane prepared with 9.9 mmol/L TMC monomer solution presents a CO 2 permeance of 81 GPU and a CO 2 /N 2 selectivity of 65, which was significantly enhanced from the non-selective supports. This work provides a facile approach for tuning the TFC membrane performance for CO 2 separation and can be extended to make high-performance membranes for industrial CO 2 capture by selecting more permeable supports.
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ACS Catalysis
·
2025
·
IF 13.1
Qianqian Song,Yingbing Zhang,Ziyang Wu,Min Kuang,Jun Chen,Jianping Yang
The electrocatalytic urea synthesis has emerged as a promising alternative strategy to replace the current energy-intensive industrial Haber–Bosch processes which are limited by sluggish C–N coupling and low selectivity because of the unmatched reduction kinetics of CO2 and nitrogen-based precursors. Herein, a thermodynamically spontaneous early stage C–N coupling pathway of *CO2 + *NO → *NOCO2 is established through the asymmetric bridging-adsorption of CO2 enabled by hydroxycarbonate-induced CO32–-Cu2+ dual sites on the tandem electrocatalyst of copper carbonate hydroxide and iron oxide grown on carbon fibers (CuCH/α-Fe2O3–CFs). This asymmetric adsorption induces a pronounced electron-deficient state of carbon atoms in CO2 due to bidirectional electron transfer toward both the CO32– and the Cu2+ centers. Coupled with the directional migration of *NO intermediates at the interface, effectively suppress the subsequent protonation of *CO2 while promoting nucleophilic attack by *NO, thereby driving spontaneous initial C–N coupling of *CO2 and *NO and significantly lowering the energy barrier of the C–N coupling step. The results demonstrate a urea Faradaic efficiency of 78.7% and urea yield rate of 1794.6 μg h–1 mgcat–1 at an ultralow applied potential of −0.20 V vs RHE, surpassing most reported catalysts to date.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Bowen Wang,Lu Song,Chen Peng,Ximeng Lv,Gengfeng Zheng
The acidic CO 2 reduction reaction (CO 2 RR) offers a promising approach to mitigate CO 2 reactant loss and carbonate deposition, which are challenging issues in alkaline or neutral electrolytes. However, the hydrogen evolution reaction (HER) competes in the proton-rich environment near the catalyst surface as a side reaction, reducing the energy efficiency of generating multi-carbon (C 2+ ) products. In this work, we proposed a palladium (Pd) doping strategy in a copper (Cu)-based catalyst to stabilize polarized Cu 0 -Cu + sites, thus enhancing the C C coupling step during the CO 2 RR while suppressing HER. At an optimal doping ratio of 6%, the Pd dopants were well dispersed as single atoms without aggregation, allowing for the stabilization of subsurface oxygen (O Sub ), preserving the polarized Cu 0 -Cu + active sites, and reducing the energy barrier of C C coupling. The Pd-doped Cu/Cu 2 O catalyst exhibited a peak Faradaic efficiency (FE) of 64.0% for C 2+ products with a corresponding C 2+ partial current density of 407.1 mA∙cm −2 at −2.18 V versus a reversible hydrogen electrode, a high CO 2 single-pass conversion efficiency (SPCE) of 73.2%, as well as a high electrochemical stability of ∼ 150 h at industrially relevant current densities, thus suggesting a potential approach for tuning the electrocatalytic CO 2 performances in acidic environments with higher carbon conversion efficiencies.
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