Energy & Environmental Materials
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2022
·Vol. 6
·期 5
·e12415
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IF 13.443
Lin Chen,Jingwen Zhou,Junxiang Zhang,Guicai Qi,Bin Wang,Jianli Cheng
High energy density Li-CO 2 batteries have attracted much attention owing to the “two birds with one stone” feature in fixing greenhouse gas CO 2 and providing renewable energy. However, poor reversibility of the discharge product Li 2 CO 3 is one of the main problems that limit its application, resulting in poor cycling stability and severe polarization. Herein, copper indium sulfide (CIS), a semiconducting non-precious metal sulfide, is fabricated as cathode catalysts for high-performance Li-CO 2 batteries. Combined with the synergistic effect of bimetallic valence bonding and coordinated electron transfer, Li-CO 2 batteries using CIS cathodes exhibit high full specific discharge capacity, excellent rate capability and cycle stability, namely it delivers a high specific full discharge capacity of 8878 μAh cm −2 , runs steadily from 10 to 100 μA cm −2 , and performs a stable long-term cycling behavior (>1050 h) under a high energy efficiency of 84% and a low charge voltage of approximately 3.4 V at 20 μA cm −2 within 100 μAh cm −2 . In addition, a flexible Li-CO 2 pouch cell is constructed to reveal the potential of employing CIS to fabricate flexible high energy storage devices in practical applications. This work shows a promising development pathway toward next-generation sustainable energy storage devices.
研究领域:
电化学
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能源材料
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纳米催化
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可持续能源存储
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金属-气体电池
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DOI
高影响因子
INORGANIC CHEMISTRY
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2019
·
IF 4.85
Changwei Chen,Xiangbo Feng,Qing Zhu,Rui Dong,Rui Yang,Yan Cheng,Chi He
In the present work, a series of MOF-74 (Ni) materials with narrow micropore channels and abundant unsaturated metal sites was respectively prepared via hydrothermal (HT), condensation reflux (CE), and microwave-assisted (MW) methods. The physicochemical properties of synthesized materials were characterized by powder X-ray diffraction, N2-sorption, field-emission scanning electron microscopy, Fourier-transform infrared (FTIR), thermogravimetric (TG)/TG-FTIR, X-ray photoelectron spectroscopy, UV–vis–near infrared, NH3/CO2-temperature programmed desorption, and in situ diffuse reflectance infrared Fourier transform spectroscopy. Their CO2/N2 adsorption performances were evaluated by isotherm adsorption and dynamic adsorption experiments. We found that the MW is a rapid and facile protocol for the synthesis of MOF-74 (Ni) materials with highly efficient CO2 capture capacity. The well-shaped MW-140 adsorbent with superior CO2 adsorption capacity of 5.22 mmol/g at 25 °C can be obtained within 60 min by the MW process, almost 6 times higher than that of the commercial activated carbon (0.89 mmol/g). Results of dynamic adsorption experiments showed that the MW-140 material possesses the highest CO2 adsorption capacity of 3.37 mmol/g under humid conditions (RH = 90%). Importantly, MW-140 has excellent adsorption stability and recyclability, superior CO2 capture selectivity (CO2/N2 = 31), and appropriate isosteric heat in CO2 adsorption (21–38 kJ/mol), making it a promising and potential material for industrial CO2 capture. Characterization results demonstrated that the high capture capability of MOF-74 (Ni) materials can be attributed to the synergistic effect of abundant narrow micropore channels and rich five-coordinated Ni2+ open metal sites which are beneficial for the trapping of CO2 molecules.
研究领域:
材料科学
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环境化学
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无机化学
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碳捕集与封存
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纳米材料
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DOI
高影响因子
INORGANIC CHEMISTRY
·
2019
·
IF 4.85
Lijia Zhou,YiFeng Han,Congling Yin,Yanhui Wang,Xiaoyan Yang,Mathieu Allix,Qingzhen Huang,Jin Xiong,Bingwu Wang,Guobao Li,Xiaojun Kuang,Xianran Xing
Topotactic reduction of the perovskite oxide TbBaCo2O5.5 with CaH2 leads to a new crystalline phase TbBaCo2O4.5, adopting a 2 × 2 × 1 superstructure compared to TbBaCo2O5.5. The structure consists of a corner-shared network of square pyramidal CoO5 and trigonal planar CoO3 units. Magnetic susceptibility and variable temperature neutron diffraction data reveal that TbBaCo2O4.5 adopts a G-type antiferromagnetically ordered structure (TN ∼ 322 K). The ordered moments are consistent with the presence of low-spin Co2+ (S = 1/2) in trigonal-planar coordination and high-spin Co2+ centers in square pyramidal coordination. TbBaCo2O4.5 shows lower conductivity than TbBaCo2O5.5, which is consistent with the p-type conduction behavior. The unique anion vacancy arrangements in TbBaCo2O4.5 further complement the role of A-cations in controlling the oxygen vacancy distribution in LnBaCo2O5+δ series and demonstrate more opportunity to tune the structural and physical properties based on cationic and anionic lattice coupling.
研究领域:
固态化学
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材料科学
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无机化学
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磁学
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晶体工程
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功能材料
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氧化物材料
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拓扑化学反应
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Ke Wang,Youwei Zhao,Peter T. Clough,Pengfei Zhao,Edward J. Anthony
Alkali metal nitrate-/nitrite-promoted MgO sorbents are promising candidates for intermediate-temperature (200–500 °C) CO 2 capture. However, the structure-performance relationship and kinetic characteristics of NaNO 2 -promoted MgO remain unclear. Here the effects of physical-chemical properties on the CO 2 sorption performance of NaNO 2 -promoted MgO and the sorption kinetics were comprehensively studied to elucidate the detailed role of NaNO 2 . Samples were characterized by X-ray diffraction, scanning electron microscopy, N 2 adsorption, Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The sorption kinetics were obtained by isothermal thermogravimetry and elucidated using a double exponential model. Compared with pure MgO and NaNO 3 -promoted MgO, NaNO 2 -modified MgO had a lower initial sorption temperature and a unique bimodal sorption characteristic. Characterization results revealed that such bimodal sorption was due to the presence of double promoters (mixture of NaNO 2 and NaNO 3 ) which implies that some of the nitrite was oxidized to nitrate during the preparation process. Deposition of double promoters further reduced the amounts of hydroxide and carbonate species for pure MgO while still preserving more hydroxide and carbonate species on the surface as compared with NaNO 3 -promoted MgO. The kinetics analysis demonstrated that the double exponential model can describe the sorption process well for both NaNO 3 - and NaNO 2 -promoted MgO, suggesting that the entire sorption occurs as a double process (surface chemisorption and product layer diffusion). Significant differences were seen from NaNO 3 -promoted MgO, and the surface chemisorption process of NaNO 2 -promoted MgO was independent of temperature, which suggests that an increased presence of hydroxide and carbonate species provides more active sites for greatly facilitating surface chemisorption.
研究领域:
材料科学
·
环境化学
·
化学工程
·
碳捕集与封存
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DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2014
·
IF 2.045
Chao Guo,Shaoyun Chen,Yongchun Zhang,Guangbo Wang
A mixture of 2-(2-aminoethylamine)ethanol (AEEA) with benzyl alcohol (BP) as absorbent was developed to reduce energy consumption in an amine-based CO2 capture process. The solubility of CO2 in the AEEA + BP solution was compared with AEEA + diethylene glycol (DEG), AEEA + triethylene glycol (TEG), and AEEA + H2O. The CO2 loading (mol CO2/kg amine) at the same CO2 partial pressure was in the order AEEA + H2O > AEEA + BP > AEEA + TEG > AEEA + DEG, and CO2 loading of all these solutions increased with increasing vapor pressure of CO2. Besides, the CO2 loading in AEEA + BP solution significantly decreased with increasing reaction temperature. The desorption rate of AEEA + BP solution was about 1.3 times faster than that of aqueous AEEA solution at the same desorption temperature, and AEEA + BP solution needed 30% time less than AEEA + H2O solution to reach reaction end point. The AEEA + BP solution showed stable repeatability in four cycles of absorption–desorption tests.
研究领域:
化学工程
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碳捕集与封存
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温室气体减排
·
分离过程
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DOI
高影响因子
Nanoscale
·
2026
·
IF 5.1
Qi Chen,Yanming Li,Hui Shi,Wenbin Ma,Chunzhen Yang,Changli Li,Jingfu He
Multi-carbon (C2+ ) products from electrocatalytic CO2 reduction (CO2 RR) hold significant industrial value. Tandem Cu-based catalytic systems can markedly improve C2+ selectivity, but their performance is often limited by suboptimal spatial configurations. In this study, we fabricate layer-stacked Ag/CuO and array-patterned Ag/CuO catalysts with tunable array spacings (200, 400, and 800 μm) to decouple CO generation and consumption, thereby enabling precise regulation of * CO flux. The array-patterned Ag/CuO systems markedly outperform layer-stacked designs, indicating that lateral CO diffusion is more effective than longitudinal diffusion.Moreover, C 2+ selectivity strongly depends on array spacing, with the best performance achieved at 400 μm (Ag-CuO-400), reaching a Faradaic efficiency (FE) of 63% for ethylene at 300 mA/cm 2 in a neutral electrolyte. Through operando infrared microscopy, we visualize the * CO coverage distribution in real time, revealing an effective lateral CO diffusion length of approximately 200 μm. This corresponds to an optimal balance between * CO supply and C-C coupling activity on the Ag-CuO-400 catalyst. This work underscores the significance of anisotropic * CO transport and provides a design strategy for spatially structured tandem catalysts.
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DOI
PubMed
高影响因子
ACS Catalysis
·
2026
·
IF 13.1
Hao Wang,Jiabao Yang,Yipu Xu,Yucai Qin,Shutao Xu,Guanghui Zhang,Zhongmin Liu,Xinwen Guo
As environmental and energy issues become increasingly apparent, the tandem catalytic hydrogenation of CO2 for direct hydrocarbon production has attracted significant attention. However, zeolite deactivation caused by metal migration severely hampers its development. This work reveals that for the In2O3/ZSM-5 catalyst in CO2 hydrogenation, indium species preferentially migrate to the external surface of ZSM-5 and interact with hydroxyl groups (e.g., Brønsted acid sites (BAS) and SiOH) via solid-state ion exchange, which is related to the subsequent poisoning of BAS within micropores. Based on this insight, a surface engineering strategy was developed by grafting silane onto the external surface, which significantly enhanced the resistance to indium poisoning. After a 22-h reaction, the silane-modified catalyst (In2O3/ZSM-5-SiPr) retained nearly all of its strong acid sites and maintained a C2+ hydrocarbon selectivity of >92.0%. However, the unmodified catalyst suffered a 60% loss of the number of strong acid sites and yielded 0% C2+ selectivity. The derived 0.6Si/In2O3/ZSM-5-SiPr achieved a C2+ selectivity of >92.0% with a space-time yield (STY) of 3.66 mmol goxide–1 h–1, which is more than 2.6 times higher than that of the reported powder-mixed In2O3 tandem catalysts, and demonstrated stability for over 260 h under harsh conditions. This strategy is generally applicable to multiple zeolites with varying Si/Al ratios and topologies. This work provides a universal approach for designing stable and highly active tandem catalysts resistant to metal migration during CO2 hydrogenation.
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产品关联
DOI
高影响因子
ACS Catalysis
·
2026
·
IF 13.1
Can Cheng,Yaolin Wang,Jia-nan Wang,Haomiao Xu,Wenjun Huang,Zhisong Liu,Wei Li,Yuyang Li,Zan Qu,Xin Tu,Naiqiang Yan
Plasma-catalytic CO2 hydrogenation to CO offers a promising route for carbon-neutral chemical synthesis. However, its advancement is constrained by low energy efficiency and limited mechanistic insight. Here, we developed an oxygen vacancy-engineered Pd-WO3–x catalyst supported on nickel foam (NF), which exhibits enhanced performance in ambient plasma-driven CO2 conversion. The system leverages the conductive properties of NF to spatially divide the discharge zone into streamer and filamentary discharge zones, thereby enhancing plasma activation and interfacial charge transfer. Catalyst characterization reveals that Pd plays a critical role in stabilizing metastable oxygen vacancies (OVs) within WO3–x, which function as electron reservoirs to promote CO2 dissociation into CO. Density functional theory calculations and in situ spectroscopic studies confirm that Pd facilitates H2 dissociation, while vibrationally excited CO2 generated in the plasma gas phase preferentially adsorbs at OV sites. At a specific energy input of 33.6 kJ L–1, the system demonstrates superior performance, achieving 54.9% CO2 conversion with 99.8% selectivity toward CO, surpassing typical plasma-catalytic benchmarks. The catalyst exhibited good stability over 100 h of continuous operation, with a slight decrease in CO2 conversion (<10%) and nearly unchanged CO selectivity (>99%) due to strong metal–support interactions and the conductive nature of NF. This work demonstrates that OV engineering provides a promising strategy for designing efficient plasma-catalytic systems for CO2 conversion.
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产品关联
DOI
PubMed
高影响因子
Scientific Reports
·
2026
·
IF 3.9
Yan Yuanzi,Tao Yan,Zhou Shaoli,Fan Yunfeng,Zhang Peng
To address the limitations of conventional CO₂-responsive plugging materials (fixed network structure, slow response, and poor long-term stability) in fractured reservoirs, a novel terpolymer hydrogel poly(acrylamide-co-2-acrylamido-2-methylpropane sulfonic-co-acid-methylenebis(acrylamide)) hydrogel, denoted as P(AM-AMPS-MDA) was designed via solution copolymerization. The hydrogel features a hybrid network of covalent crosslinks (from MDA with tunable ethyleneamino chain length n = 1–3) and CO₂-induced ionic clusters, with precise reactant ratios (AM: AMPS: MDA = 90:16:4, K₂S₂O₈:Na₂SO₃=2:1) ensuring reproducibility. Comprehensive characterizations (FTIR, TGA/DSC, rheology, strain sweep) confirmed its superior performance: the optimized MDA₂ hydrogel ( n = 2) exhibits rapid CO₂ response (< 10 min), balanced swelling ratio (~ 18), high storage modulus (1790 Pa), and excellent thixotropy (> 90% recovery in 30 s). It maintains structural integrity at 80 °C ( T d ≈ 617 °C) and retains > 85% mass over 10-year reservoir simulation. Core flooding tests and visual demonstrations validate its effective plugging (residual resistance coefficient > 20) and injectability. This design resolves key trade-offs in existing systems, providing a promising candidate for conformance control in CO₂-enhanced oil recovery and sequestration.
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 4.3
Ling Chen,Xiangyu Ma,Tingting Wang,Qingliang Li,Ruru Qian,Mengting Cui,Haizhu Yu,Manzhou Zhu
The atomic precision of metal nanoclusters reveals their size-dependent physicochemical properties and highlights the challenges in achieving controllable synthesis at the single-atom level. Herein, we report a series of silver clusters adopting an atom-by-atom evolution pattern, including Ag 13 (SR 1 ) 12 (DPPP) 3 , Ag 14 (SR 1 ) 12 (DPPF) 3 , and Ag 15 (SR 1 ) 12 (DPPB) 3 (Ag 13 -Ag 15 , HSR 1 and DPPP/DPPF/DPPB denote 3,5-bis(trifluoromethyl)thiophenol, and 1,3-bis(diphenylphosphino)propane/ferrocene/butane). Each of these three clusters comprises a shell structure with three groups of Ag 2 (SR 1 ) 4 (DPPX) (X=P/F/B) blocks, while the metallic core corresponds to singly, linearly, and triangularly capped distorted octahedral Ag 6 structures. So far, Ag 13 represents the first 1e metal cluster. The kinetic monitoring and the molecular dynamic (MD) simulations demonstrate the nucleation driven by ligand flexibility. The structural peculiarities of the nanoclusters (which are loaded on activated carbon) govern their divergent catalytic behaviors in epoxide carboxylation reactions. The DPPF stabilized Ag 14 cluster exhibits high activity (98 % yield in 20 h at 75°C, and well maintained after 5 cycles), outperforming Ag 13 (56 %) and Ag 15 (65 %) under otherwise identical conditions. The DFT results show that CO 2 could be significantly stabilized by parallel benzene rings around AgS 2 in Ag 14 , forming π-CO 2 -π structures. This study establishes a dual structure–activity relationship: ligand flexibility regulates the nucleation process during synthesis, whereas the resultant surface defects induced by rigid ligands determine catalytic performance.
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.3
Xuejian Liu,Zhenyuan Yin,Jiayu Sun,Xinrui Cai,Yan Li,Guangjin Chen,Chenlu Xu,Hongfeng Lu,Praveen Linga
Achieving global net-zero emissions necessitates advancements in sustainable CO2 sequestration technologies. CO2 sequestration in subsea sediments in the form of clathrates presents a promising option due to inherent reaction conditions, high CO2 storage capacity, and superior stability. However, the sluggish CO2 hydrate formation kinetics significantly constrains its field-scale application, particularly in the process of CO2 hydrate cap formation to prevent the CO2 leakage. Herein, we propose a biomolecular strategy by using the low-dose hydrophobic amino acid l-methionine to address this challenge. Combining morphological imaging and in situ Raman spectroscopy, l-methionine was found to disrupt the rigid CO2 hydrate films and induces self-organized liquid CO2 transport channels, significantly reducing CO2 mass transfer resistance. Molecular-level analysis further reveals that the hydrophobic group of l-methionine leads to a 70% decrease in the energy barrier of the CO2 diffusion. This biocompatible promoter enables ultrahigh CO2 uptake (120.6 v/v) with a 15-fold enhancement over pure water. Rapid CO2 hydrate formation for hydrate-sediment cementation was further validated using the acquired South China Sea clayey-silty marine sediments. This environmentally benign strategy demonstrates extraordinary CO2 hydrate formation kinetics from liquid CO2 compared to the state-of-the-art promoters, offering a promising and practical solution for long-term offshore CO2 storage to mitigate climate change.
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.7
Guoqiang Hou,Di Xu,Haifeng Fan,Yangyang Li,Siyi Huang,Mingyue Ding
Direct synthesis of dimethyl carbonate (DMC) from CO 2 is critical for achieving carbon neutrality, yet the sluggish formation and conversion of the key *CH₃OCOO intermediate-due to the difficulty of C-O coupling-limit high DMC yields. Herein, we developed a boric acid-assisted recrystallization strategy to fabricate grain-boundary-rich CeO 2 hollow nanospheres, which serve as an efficient catalyst for CO 2 to DMC synthesis. The introduction of grain-boundary (GBs) induced the electron redistribution, which led a decrease in the electron density of bulk Ce ions and created a localized electron-rich region at homogeneous interface. This unique electronic landscape promoted reactive methoxy formation and stronger CO 2 adsorption, thereby enabling more efficient coupling of *CH 3 O and *CO 2 to form the *CH 3 OCOO. Concurrently, the enhanced CO 2 adsorption facilitated the dissociation of *CH 3 OCOO and subsequent DMC formation. As a result, the 4%BCeO 2 -GBs achieved an advantageous DMC yield of 19.8 mmol/g. In the assistance of dehydrating agent, the catalyst delivered a remarkable 264.2 mmol/g DMC yield and 7.12% methanol conversion, which was 32 times higher than commercial CeO 2 . This study elucidated the intrinsic mechanisms governing *CH 3 OCOO intermediate behavior and offers valuable guidance for CO 2 converting into high-value organic chemicals.
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）