Nature Communications
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2024
·Vol. 15
·期 1
·1-11
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IF 14.7
Li Wei,Zhang Menghang,Sun Xinyi,Sheng Chuanchao,Mu Xiaowei,Wang Lei,He Ping,Zhou Haoshen
Li-CO 2 batteries offer a promising avenue for converting greenhouse gases into electricity. However, the inherent challenge of direct electrocatalytic reduction of inert CO 2 often results in the formation of Li 2 CO 3 , causing a dip in output voltage and energy efficiency. Our innovative approach involves solid redox mediators, affixed to the cathode via a Cu(II) coordination compound of benzene-1,3,5-tricarboxylic acid. This technique effectively circumvents the shuttle effect and sluggish kinetics associated with soluble redox mediators. Results show that the electrochemically reduced Cu(I) solid redox mediator efficiently captures CO 2 , facilitating Li 2 C 2 O 4 formation through a dimerization reaction involving a dimeric oxalate intermediate. The Li-CO 2 battery employing the Cu(II) solid redox mediator boasts a higher discharge voltage of 2.8 V, a lower charge potential of 3.7 V, and superior cycling performance over 400 cycles. Simultaneously, the successful development of a Li-CO 2 pouch battery propels metal-CO 2 batteries closer to practical application.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Hongyuan Chuai,Haibei Yang,Sheng Zhang
Ni single-atom-decorated nitrogen-doped carbon materials (Ni–Nx-C) have demonstrated high efficiency in the electrochemical reduction of CO2 (CO2RR) to CO. In this study, Ni–Nx-C active sites were embedded within a carbon membrane via an electrospinning and pyrolysis process. The resulting self-supported carbon membrane hosting Ni–Nx-C sites could be directly utilized as an electrode for the CO2RR. To enhance the CO2RR performance of the carbon membrane, the porous structure of the carbon membrane was fine-tuned by incorporating a pore-forming agent. The optimized porous carbon membrane electrode, K0.66-Ni-NC, achieved an impressive CO faradaic efficiency (FECO) of over 90% within a wide potential range from −0.8 to −1.6 V vs RHE for CO2RR. Additionally, it maintained an FECO of above 90% at −0.8 V vs RHE throughout a 30 h durability test in an H-cell. Further analysis has revealed that the porous structure of the carbon membrane not only facilitates the mass transport of CO2 but also increases the level of exposure of active sites during the CO2RR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Fu Li,Qian Huo,Xiaomei Zhou,Shasha Fang,Fei Han,Jingnan Yang,Qingxin Guan,Wei Li
Photothermal CO 2 into methanol is an effective approach to address energy and environmental challenges, but the low conversion and poor selectivity limit its large-scale application. Here, 0.5Cu@CeO 2 with atomically dispersed active sites and abundant Frustrated-Lewis-pairs (FLPs) was synthesized using coordination complex precipitation reaction. The substitution of Cu 2+ with Ce 3+ results in the formation of new FLPs, which promotes the upward shift of conduction band (CB) and enhances the reducing capability of catalyst. Moreover, the more sensitive and stronger capability of photogenerated carriers also endows 0.5Cu@CeO 2 with stronger CO 2 reduction capability. The photothermal methanol yield of 0.5Cu@CeO 2 reached 1896.02 μmol·g cat –1 ·h –1 . The DFT results demonstrate the FLPs structure of 0.5Cu@CeO 2 promotes parallel adsorption of CO 2 and *CO species. Meanwhile, the presence of O v inhibits the dissociation of oxygen species, consequently boosting the methanol synthesis. The construction of FLPs structure introduces a novel method to enhance CO 2 conversion utilizing photothermal catalysis.
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MATERIALS LETTERS
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2024
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IF 2.7
Hongmin Cui,Jianguo Xu,Nanfu Yan,Runhan Yan,Jinsong Shi
In the current work, we explored the direct synthesis of S-doped porous carbons employing cesium methanesulfonate as a novel bifunctional chemical activator. The obtained carbons showed high surface area (654–2264 m 2 /g) and high S content (6.56–15.13 wt%). Effects of activation temperature and cesium methanesulfonate amount on the carbons’ properties were also studied. The obtained carbons showed CO 2 uptake of 3.58–4.76 mmol/g at 0 °C and 1 bar. Effects of textural properties and S-doping on CO 2 adsorption performances were discussed.
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AICHE JOURNAL
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2025
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IF 4
Hui Wang,Yifan Jin,Yaxin Jin,Siyu Kuang,Tianxiang Yan,Xinyue Wang,Xiao Wang,Wenquan Cui,Sheng Zhang
Electrochemical carbon dioxide reduction reaction (CO 2 RR) is one of the most prospective strategies to achieve carbon neutrality. Multi-carbon compound (C 2+ ) products have higher commercial value and wider applications, among which ethanol is a widely used chemical feedstock and high energy density fuel. Here, we prepared nitrogen-doped carbon nanofibers containing copper-zinc double atoms using the electrospinning technique and controlled the content of both metal atoms by varying the calcination temperature. This catalyst exhibited ultra-high selectivity for ethanol at low potentials. Ethanol selectivity at −0.3 V versus RHE was more than 60% with the total alcohol selectivity of over 80%. Meanwhile, we explored the ethanol production pathway by combining density-functional theory (DFT) and ATR-FTIR spectroscopy, and found that OCCO* intermediates were most abundant for the optimal ratio of Cu to Zn atoms, lowering the energetic barriers to ethanol formation, and thus improving the selectivity of ethanol production.
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Small
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2025
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IF 12.1
Ruipeng Jin,Rui Li,Ming-Li Ma,Da-Yu Chen,Jian-Yu Zhang,Zheng-He Xie,Li-Feng Ding,Yabo Xie,Jian-Rong Li
Metal–organic frameworks (MOFs) are rigorously investigated as promising candidates for CO 2 capture and conversion. MOF-on-MOF heterostructures integrate bolstered charger carrier separation with the intrinsic advantages of MOF components, exhibiting immense potential to substantially escalate the efficiency of photocatalytic CO 2 reduction (CO 2 RR). However, the structural and compositional complexity poses significant challenges to the controllable development of these heterostructures. Herein, a conventional MOF-on-MOF nanocomposite is readily optimized from a type II heterojunction to a state-of-the-art cascade Z-scheme configuration via the encapsulation of Pt nanoparticles (Pt NPs), establishing synergistic MOF-MOF and metal-MOF heterojunctions with reinforced built-in electric field. A cascade electron flow is thus propelled, vigorously separating the photogenerated charge carriers and profoundly extending their lifetimes. Collectively, the photocatalytic activity of the cascade Z-scheme is drastically promoted, exhibiting a nearly quintuple enhancement in the CO production rate over the original type II heterostructure. Moreover, the anti-sintering capacity of the developed nanocomposite is unveiled, elucidating its simultaneously improved activity and stability. These findings present unprecedented regulation over the configuration of a MOF-on-MOF heterojunction, substantially enriching the fundamental understanding and rational design strategies of composite materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Xiaohong Ma,Huacheng Jin,Fei Li,Yuanjiang Dong,Dan An,Danyang Li,Jian Qi,Feifei You,Ming-shui Yao,Fangli Yuan
Although ZnO has potential application in photocatalytic CO 2 reduction, it faces challenges such as limited light absorption range and high recombination of photo-induced electron/hole pairs. Given this, it is necessary to continuously explore new design strategies and optimization approaches to improve the performance of ZnO in photocatalytic CO 2 reduction. In this work, ZnO nanorods (NRs) doped with Cu, Fe, and co-doped Cu/Fe are successfully synthesized through chemical displacement reaction obtaining precursors of uniformly dispersed dopants and subsequent treatments of radio-frequency (RF) thermal plasma technology. The effects of doping species and amounts on the oxygen vacancies and photocatalytic performances of ZnO are systematically investigated. The results indicate that (i) the introduction of metal cation dopants can effectively reduce the intrinsic band gap structure of ZnO, leading to broaden light absorption range in the visible light region and improving light utilization efficiency and (ii) the defects introduced by doping suppress the recombination of photo-generated charge carriers. The synergistic effect of the two aspects improves the photocatalytic activity in CO 2 reduction. Especially, the bimetallic co-doped sample possesses much more oxygen vacancies with a bandgap of 2.71 eV, exhibiting optimal photocatalytic performance and cycling stability. This study has brought breakthroughs and progress in the field of photocatalytic CO 2 reduction, including but not limited to, expanding the synthesis and regulation strategies of metal oxide semiconductor photocatalysts.
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Catalysis Science & Technology
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2024
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IF 4.4
Xuewei Tu,Can Sun,Yang Hu,Yutong Chen,Shouxin Zhu,Jingyi Qu,Zhexiao Zhu,Xiang Zhang,Hui Zheng
Cycloaddition of CO2 and epoxides to synthesize cyclic carbonates via photothermal catalysis represents one of the effective strategies for achieving carbon neutrality. In this study, a facile one-step hydrothermal method was employed to synthesize a bimetallic photothermal catalyst FeCo@BPDC. This catalyst demonstrates remarkable efficiency in fixing CO2 to synthesize cyclic carbonates under atmospheric pressure and solvent-free conditions. Through comprehensive characterization and experimentation, the indispensability of bimetallic active sites has been convincingly demonstrated. Additionally, the incorporation of organic ligands significantly enhances the concentration of oxygen vacancies within the catalyst, thereby endowing it with excellent photocatalytic performance. This study presents a novel perspective for the design of photothermal catalysts that convert CO2 into value-added chemicals under mild conditions.
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CHEMISTRY OF MATERIALS
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2025
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IF 7
Beibei Sun,Cheng Zeng,Suyun Deng,Yuewen Gu,Lei Gan,Huajun Yang
The separation of C2H2/CO2 under highly humid conditions by using metal–organic frameworks (MOFs) is extremely challenging because water vapor would reduce the C2H2 adsorption capacity or even degrade the structure of MOFs. In this work, a zirconium zeolitic metal–organic framework (NNM-5) with a small aperture and large cavities exhibits commendable C2H2/CO2 selectivity (16.6 at 298 K and 1 bar) and a high uptake ratio (3.13 at 298 K and 1 bar). More importantly, NNM-5 could maintain at least five breakthrough cycles under highly humid conditions (around 100% RH) without performance degradation compared to that under dry conditions. Our studies indicate that the kinetic mechanism is the key to excellent separation performance under highly humid conditions based on the fact that the material is hydrophilic with a high water uptake, but the diffusion rate of H2O is 2 orders slower than that of C2H2 and CO2 in NNM-5.
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Journal of Materials Chemistry A
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2025
·
IF 9.5
Tao Zhang,Ruijia Wang,Wei Li,Shujun Li,Bing Tian,Shouxin Liu,Zhijun Chen
A simple carbon dots (CDs) catalyst prepared from lignin-derived syringic acid was used for catalytic fixation of CO2 with epoxides to synthesize cyclic carbonates. The catalysts exhibited high catalytic performance which can proceed the reaction under metal-, solvent-, halogen-, and additive-free conditions with 1 atm of CO2 and 80 °C reaction temperature. Various cyclic carbonates could be obtained in high yields and selectivities under the extremely mild catalytic conditions. Additionally, the CDs catalysts showed excellent recyclability with stable catalytic activity. Mechanistic study revealed that the hydroxyl groups on the surface of CDs are responsible for epoxides activation and nitrogen-containing sites (graphitic N and pyridinic N) are crucial for CO2 activation. The cheap precursors, easy and sustainable preparation of catalyst, mild and simple operation of CO2 fixation make the CDs catalyst a promising catalyst for the CO2 conversion.
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Catalysis Science & Technology
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2024
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IF 4.4
Zafar A. K. Khattak,Nazir Ahmad,Hussein A. Younus,Habib Ullah,Baoyi Yu,Khurram S. Munawar,Muhammad Ashfaq,Muhammad Yaseen,Muhammad Danish,Mohammed Al-Abri,Rashid AlHajri,Francis Verpoort
Metal(II)-carboxylate frameworks are an important class of MOF materials finding applications in gas storage, separation, sensing, catalysis, etc. Recently, their design, synthesis and characterization have been established at a very fast pace. Here two novel MOFs based on 5,5′-(([1,1′-biphenyl]-4,4′-dicarbonyl)bis(azanediyl))diisophthalic acid (H4L, an amide containing ligand) and transition metals (copper and zinc) are reported. Several characterization tools e.g., FT-IR, XRD, SEM, TGA, and XPS are used to characterize these MOFs. Single-crystal X-ray diffraction and Hirshfeld surface analyses are used to characterize the 3D structural framework. The void and cavity analysis revealed the strength of the crystal packing. Both MOFs followed multistage thermogravimetric disintegration profiles. The solvent molecules escaped around 200 °C and the structural changes due to decompositions in the frameworks continued till 500 °C. The morphological analysis for Zn-MOF and Cu-MOF showed uniform wedge-shaped rectangular blocks and spherical balls with dimensions around 100 and 50 μm, respectively. The amide functionalized Zn(II)-carboxylate framework exhibited high catalytic activity (85–>99%) towards the solvent-free cycloaddition of CO2 to different epoxides e.g., epichlorohydrin, propylene oxide, allyl glycidyl ether and glycidyl isopropyl ether with 100% selectivity under ambient conditions (i.e., 1 bar at 40 °C for 24 h) at very low catalyst loading. By adjusting the reaction conditions (T, P, and co-catalyst), the catalytic conversion reached 100% within only 2 hours. The results showed Zn-MOF as a superior and efficient catalyst compared to other reported MOFs. Additionally, the catalyst can be easily recovered and regenerated for repeated use without performance loss.
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BIORESOURCE TECHNOLOGY
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2025
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IF 9
Chun Yang,Lei Mao,Yaxin Chen,Yanhong Zhou,Ruifang Zhang,Zhiwei Yi,Dechao Zhang,Guangya Zhang
Carbonic anhydrases (CAs) has garnered increasing attention in carbon capture, utilization and storage (CCUS) due to their ecological friendliness. However, most of them suffer susceptibility to deactivation in harsh conditions. Herein, a reliable dataset was adopted for creating ancestral CAs through an optimized ancestral sequence reconstruction (ASR) method. After prescreening, the ancestor AncCA19 was obtained and successfully expressed. The hydration activity of AncCA19 was as high as 58,859 WAU/mg, with the optimum temperature and pH obtained by esterase assay at 100 ℃ and 9, respectively. AncCA19 had the longest half-life (1.7 h) at 95 ℃ compared with existing CAs. After 2 weeks’ incubation in artificial seawater at 30 ℃ or 25.0 % N-methyldiethanolamine (MDEA) at 60 ℃, the activities remained above 47,370 WAU/mg and 6,596 WAU/mg, respectively. Thus, AncCA19, as a novel benchmark of CAs, exhibits exceptional stability in a variety CCUS applications, establishing a versatile candidate for effective CO 2 capture.
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