APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Ming-Dong Xie,Jia-Meng Sun,Zhong-Hua Zhang,Hong-Qing Liang,Zhi-Kang Xu
Electrochemical CO 2 reduction (CO 2 RR) in acidic media circumvents carbonate crossover and salt precipitation inherent to alkaline and neutral systems, but suffers from low selectivity due to the dominance of hydrogen evolution. While alkali cations suppress proton activity, they inevitably lead to catastrophic (bi)carbonate deposition and electrode flooding. Here, we decouple CO 2 RR from alkali cations by constructing a micro-alkaline catalytic environment using a proton-blocking hydrophobic membrane with tethered cations. We designed a series of quaternized copolymers from dimethylaminoethyl methacrylate and lauryl methacrylate (qDMA-n), where the “cation–hydrophobicity balance” was precisely tuned to optimize the balance between Donnan exclusion and water management. Integrated into a zero-gap membrane electrode assembly electrolyzer, the optimized membrane enabled CO 2 RR on Ag catalysts with a CO faradaic efficiency of 96.9 % and a single-pass conversion efficiency of 92.4 % at 200 mA cm⁻ 2 in pure 0.05 M H 2 SO 4 , maintaining stable operation for over 100 h. Finite element simulations, rotating disk electrode tests and in-situ Raman spectra revealed that the balance between cationic and hydrophobic domains plays a key role in forming a stable micro-alkaline interface despite bulk acidity, leading to effective HER suppression. This work provides a practical and generalizable interface design principle for efficient CO 2 electrolysis in strong acids, offering new opportunities for durable, high-efficiency CO 2 electrolyzers without alkali cations.
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Journal of Physical Chemistry C
·
2025
·
IF 3.2
Chuyi Zhang,Jiaxin Liu,Zhi Sun,Yuning Liang,Qun Xu
With the development of spintronics, ferromagnetic nanomaterials have shown unique advantages in the fields of information storage and quantum computation. The ABO3-type perovskite oxide ZnSnO3 is expected to realize d0 ferromagnetism due to its tunable crystal structure and unique electron arrangement. In this work, for the first time, the inhomogeneous oxygen octahedral structural distortion along the c-axis induced by SC CO2 can be found in 2D ZnSnO3, i.e., distortion of ZnO6 is larger than that of SnO6, and they are served as the structural basis for the generation of room-temperature ferromagnetism. In addition, combining the change in the concentration of the oxygen vacancies to ultimately realize the room-temperature d0 ferromagnetism in ZnSnO3 (Tc = 400 K, Ms = 0.1123 emu/g) can be presented. Therefore, this study establishes a new strategy for the development of transition metal-free ferromagnetic materials for the application of spintronic devices at room temperature.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Zhi-Wen Wang,Qiang Wan,Ying-Zhang Shi,Huan Wang,Yue-Yue Kang,Shu-Ying Zhu,Sen Lin,Ling Wu
Ultrathin TiO 2 nanosheet (NST) with abundant Ti 3+ sites is developed as a photocatalyst which exhibits a high yield (147.2 μmol g −1 h −1 ) and selectivity (96.8%) for CO 2 to CH 4 . The results of in situ FTIR, in situ EPR and density functional theory (DFT) calculation suggest that CO 2 would be selectively activated on NST surface via forming the bridging Ti···CO 2 − ···Ti coordination species which not only lowers the activation energy barrier, but also determines the selectivity of CH 4 . Additionally, NST with the better separation and transfer ability for photogenerated electrons-holes can fleetly supply the electrons to CO 2 molecules for high efficiently producing CH 4 via the Ti-C coordination bond. Finally, a possible mechanism of the synergistic effect about coordination-activation and photocatalysis is discussed at a molecule level. This work would offer a perspective for designing an effective photocatalyst and tailoring the selectivity of products by coordination activation.
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CATALYSIS COMMUNICATIONS
·
2024
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IF 3.4
Zhi-Gang Hu,Lichun Li,Shui-Bao Yu,Zhengfei Chen,Jian-Quan Weng
Several tertiary amine solutions with different structures were tested in the integrated CO 2 capture and hydrogenation process in the presence of heterogeneous Pd/NAC catalysts. The tertiary amines of 3-dimethylamino-1,2-propanediol (3DMA-1,2-PD) and 3-diethylamino-1,2-propanedio (3DEA-1,2-PD) with high CO 2 absorption capacity and high formate yield were selected as suitable candidates as CO 2 capture and hydrogenation solvents. Under mild reaction conditions, a high formate yield of 68% was achieved when using 1 M 3DMA-1,2-PD solution with CO 2 loading of 0.5 mol amine/mol CO 2 . In addition, the physico-chemical properties of the Pd/NAC catalysts were examined and the reaction mechanism of CO 2 absorption and hydrogenation in the presence of Pd/NAC was proposed.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Yanduo Liu,Mengwei Li,Jianing Guo,Ge Jin,Yue Yin,Yu Cui,Tong Sun
Recently, there has been a significant increase in interest in using photocatalysis for the energy conversion of polluting gases. In this research, sodium and ruthenium bimetallic functional sites co-modified bismuth tungstate (Ru/Na-Bi 2 WO 6 ) nanoflower photocatalyst was synthesized via the hydrothermal method. The CO 2 reduction products on the Bi 2 WO 6 substrate were CO (1.66 μmol/g/h, 68 %) and CH 4 (0.78 μmol/g/h, 32 %). After optimization, a significant change in the CO 2 products of the Bi 2 WO 6 -based composite material was observed, with CO (0.61 μmol/g/h, 3.6 %) and CH 4 (16.1 μmol/g/h, 96.4 %). Results showed that the dominance of CH 4 as the main product in the Ru/Na-BWO system is attributed to the effective doping of Na, which generates impurity energy levels composed of oxygen vacancies, lowering the conduction band position of Bi 2 WO 6 , thereby suppressing CO generation, and enhancing CH 4 selectivity by changing the CO 2 activation pathway. The remarkable performance is ascribed to the synergized adsorption and activation of CO 2 by the tandem Na + sites and Ru 0 sites. Specifically, the doped Na + sites play a major role in promoting the adsorption CO 2 molecules, while the Ru 0 sites play a dominant role in facilitating the activation of the intermediates.
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PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
He Xiaoyang,Lin Li,Li Xiangying,Zhu Minzhi,Zhang Qinghong,Xie Shunji,Mei Bingbao,Sun Fanfei,Jiang Zheng,Cheng Jun,Wang Ye
The membrane electrode assembly (MEA) is promising for practical applications of the electrocatalytic CO 2 reduction reaction (CO 2 RR) to multi-carbon (C 2+ ) compounds. Water management is crucial in the MEA electrolyser without catholyte, but few studies have clarified whether the co-feeding water in cathode can enhance C 2+ formation. Here, we report our discovery of pivotal roles of a suitable nanocomposite electrocatalyst with abundant Cu 2 O−Cu 0 interfaces in accomplishing water-promoting effect on C 2+ formation, achieving a current density of 1.0 A cm −2 and a 19% single-pass C 2+ yield at 80% C 2+ Faradaic efficiency in MEA. The operando characterizations confirm the co-existence of Cu + with Cu 0 during CO 2 RR at ampere-level current densities. Our studies reveal that Cu + works for water activation and aids C‒C coupling by enhancing formations of adsorbed CO and CHO species. This work offers a strategy to boost CO 2 RR to C 2+ compounds in industrial-relevant MEA by combining water management and electrocatalyst design.
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PubMed
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Molecular Catalysis
·
2024
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IF 3.9
Chi Ma,Zhiyong Zhong,Quanjun Xiang
The photocatalytic efficiency of bismuth-based metal-organic framework (Bi-MOF) is extremely restricted by the rapid recombination of photogenerated electron-hole pairs, which reduce the number of electrons involved in the photocatalytic reduction reaction. Constructing precise interfacial bond bridges between metal nanoparticles (NPs) and MOFs has emerged as an effective strategy to address the above-mentioned issues, promoting the electrons transfer. Herein, this study improves the sluggish dynamics of photogenerated charge in Bi-MOF by inducing the Pd-O-Bi bond bridges at the interface on a Pd NPs-decorated Bi-MOF (Pd/Bi-MOF) nanosheets. This phenomenon results in an interaction between Pd NPs and the Bi-MOF support. And Pd-O-Bi bond bridges provide the fast electron transfer channels, triggering the directional migration of photogenerated electrons from Pd to Bi node, then enhancing the spatial separation of photogenerated electron-hole pairs, finally facilitating overall photocatalytic CO 2 reduction. The presence of these bond bridges leads to higher enhancement in CO production for Pd/Bi-MOF nanosheets compared to the Bi-MOF nanosheets under visible light irradiation after 4.5 h. This research demonstrates the importance of interfacial bond bridges and provides a reasonable guide to design efficient photocatalyst for reduction of CO 2 to CO.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 28
·17181-17192
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IF 10.7
Chen Yu,Taoning Lei,Li Xu,Chuyao Jin,Jundong Yi,Shenghui Liu,Saisai Lin,Yang Yang,Hao Song,Kaige Wang,Haidong Fan,Chenghang Zheng,Xiao Zhang,Xiang Gao
Establishing a suitable electrode microenvironment is important to achieving high-efficiency electrocatalytic CO2 reduction at industrially relevant current densities. Introducing ionomers provided an effective method for regulating the electrode microenvironment, but the mechanism of interactions between the ionomer and the catalyst remains elusive. In this work, the influence of three types of ionomers on the performance and microenvironment of Ag nanoparticle (NP) and molecularly dispersed cobalt phthalocyanine (CoPc MDE) catalysts were systematically investigated. It was found that the non-covalent interactions between the ionomers with aromatic groups and CoPc MDE resulted in the hydrophilicity of electrode and undesirably promoted the generation of hydrogen during the reaction. The optimal ionomer–catalyst combinations achieved excellent FE(CO)s > 99% at current densities up to −200 mA cm−2 and stable operation for more than 180 h at a current density of −100 mA cm−2. This work underlines the necessity of selecting appropriate ionomer according to the nature of catalyst.
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AICHE JOURNAL
·
2024
·
IF 3.5
Xueqi Sun,Shaojuan Zeng,Guilin Li,Yinge Bai,Minghua Shang,Jian Zhang,Xiangping Zhang
The selective separation of CO 2 from CH 4 -containing gases is crucial to produce clean energy gases. In this study, triazole anion-functionalized ionic liquids (TAFILs) were designed by combining low molecular weight cations with triazole anions containing N electronegative site and further mixed with physical solvents to form physicochemical absorbents. The results indicated that [Cho][Triz]/TMS (80 wt%/20 wt%) not only absorbs 0.125 g CO 2 /g absorbent equal to that of 30 wt% MEA solution at 40°C and 1 bar, but also has low enthalpy of −35.76 kJ/mol less than half of 30 wt% MEA solution. Simultaneously, a super high CO 2 /CH 4 selectivity of 191.0, higher than most of the reported absorbents, is obtained for [Cho][Triz]/TMS solvents. Such great performance of CO 2 separation was attributed to relatively weak chemical and physical interaction between CO 2 and TAFIL binary absorbents. This study may provide novel promising ionic liquid absorbents for CO 2 capture applications from clean energy gases.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2024
·
IF 2.7
Wei Zhao,Hongjing Liu,Chengpeng Zhang,Yuyang Cao,Yuying Xu,Xueli Liu,Zhen Lu
Metal–organic frame UiO-66-NH 2 was modified by 3-glycidyl ether oxypropyl trimethoxysilane (KH560), and KH560-UiO-66-NH 2 was synthetized and added to Pebax to prepare KH560-UiO-66-NH 2 /Pebax mixed matrix membranes (MMMs). The epoxy group of KH560 had an amine-epoxidation reaction with the NH 2 in UiO-66-NH 2 , which prevented UiO-66-NH 2 from agglutinating in the MMMs. In addition, the N H bond and OH bond of KH560-UiO-66-NH 2 could theoretically form hydrogen bonds with CO and N H bonds in the main chain of polymerization, respectively, so as to improve the interfacial compatibility between fillers and polymers. The structure and properties of the filler particles and MMMs were evaluated by Fourier transform infrared spectrometer, x-ray diffraction, scanning electron microscopy, and thermogravimetric analyzer. The results showed that the filler particles were successfully synthesized, and had good crystallinity, uniform size distribution, and good thermal stability. The inorganic and organic interfaces of MMMs had no obvious interface defects. The obtained KH560-UiO-66-NH 2 /Pebax MMMs showed CO 2 permeability of 111.52 Barre and CO 2 /N 2 selectivity of 92.16, which were 85.65% and 88.73% higher than that of pristine membranes, respectively. The gas separation performance of MMMs was significantly improved, exceeding the upper bound of 2008 Robeson.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Xiaoyuan Luo,Zhenze Han,Xuetian Guo,Yu Wei,Yan Gao
Bismuth-based metal–organic frameworks (MOFs) have shown promise in the electrocatalytic CO2 reduction reaction (ECO2RR) due to their abundant active sites and high selectivity. In this study, microfluidic synthesis technology was innovatively introduced to achieve the continuous synthesis of the bismuth-based MOF material CAU-17. Compared with the hydrothermal method, by adjusting the flow rate while keeping the temperature and Bi3+ reaction concentration constant, the particle size and morphology could be effectively controlled, and the synthesis time was reduced to 1/36 of that of the traditional method. CAU-17 particles with different sizes showed different reactivity sensitivities to the ECO2RR. CAU-17-F60 with the smallest particle size showed the highest Faraday efficiency of 92.79% for formate at −1.2 VRHE, along with a larger electrochemically active surface area and lower interfacial resistance. It could be electrolyzed stably for 12 h, during which the average FEformate remained above 90% all the time. This study thoroughly demonstrates the significant potential of microfluidic technology in the precise control of fine structures and performance optimization of MOF catalysts, offering a new idea and a generalizable path for the sustainable preparation of efficient ECO2RR catalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Linglong Wang,Bangyan Zhang,Yang Song,Tao Gan,Jiansong Miao,Peng Zhang,Jingjing Jiang,Chunming Xu,Xiaohui Sun
Nitrogen-doped carbon nanoparticle-supported single-iron-atom catalysts (denoted as Fe-N-C) have been widely investigated in the electrocatalytic CO2 reduction reaction (CO2RR). However, for most Fe-N-C catalysts fabricated via high-temperature pyrolysis, abundant active Fe sites are buried in the bulk of microporous carbon substrate, with poor accessibility. The morphology limitation immensely alleviates the exposure of active sites at the critical three-phase interfaces and hinders the mass transfer of reactant molecules within electrodes. Herein, we present a facile soft-template coating approach to fabricate a core–shell Fe-N-C catalyst with highly accessible Fe sites at the surface by pyrolysis of an iron-coordinated polydopamine-coated ZIF-8 composite precursor. The unique core–shell structure of Fe-N-C shortens the diffusion path of ions and CO2, and it facilitates CO product elimination. Such an electrode assembly significantly boosts the electrocatalytic CO2RR in a gas-diffusion-electrode with a CO Faradaic efficiency (FECO) of ∼97% at an industrial current density of 100 mA/cm2. This work sheds light on the synthesis of single-atom catalysts with highly accessible active sites in surface layers for the CO2RR and other electrocatalytic reactions with high activity and efficient mass transport.
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