Exploration
·
2026
·
IF 30.4
Ruijia Wang,Hongda Guo,Tao Zhang,Xiaoxia Chen,Min Ge,Shujun Li,Jian Li,Bing Tian,Bernd Strehmel,Shouxin Liu,Andrey L. Rogach,Tony D. James,Zhijun Chen
Fixation of CO 2 through photocatalytic cycloaddition with epoxides to synthesize cyclic carbonates is an important but challenging process. In this work, carbon dots (CDs) synthesized from gallic acid and polyethylenimine are used for the efficient catalytic cycloaddition of CO 2 with epoxides in the absence of any solvent, additives, and halides, and importantly upon irradiation by natural sunlight. Specifically, carbon dots generated thermal energy and electrons upon solar irradiation, which together with their surface N-sites activated the inert CO 2 . Meanwhile, epoxides were activated by the surface hydroxyl and carboxylic groups of the carbon dots, which reacted with activated CO 2 at solar thermal-induced high temperatures. The CDs shows excellent stability and recyclability during the catalysis. A 1000 mmol scale reaction for cyclic carbonate synthesis performed well upon irradiation with natural sunlight in the presence of CDs, showing great potential for the industrial application due to the simple, mild, and energy-saving process.
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PubMed
高影响因子
ACS Catalysis
·
2026
·
IF 13.1
Jiejie Ling,Jilong Wang,Yao Xiao,Yan Gao,Xudong Tian,Jie Tuo,Chuang Liu,Dunru Zhu,Jingang Jiang,Shipeng Ding,Jian Li,Zhendong Wang,Anmin Zheng,Peng Wu,Le Xu
The conversion of CO2 to hydrocarbons via the methanol-mediated pathway represents a crucial route for carbon neutrality, yet preferable production of more value-added light olefins remains constrained by the fundamental activity-selectivity trade-off in zeolite catalysts. While previous studies established an acidity regulation mechanism based on balancing acid density with acid strength, the conversion of methanol intermediates is also critically governed by their intracrystalline diffusion, which can be severely hindered by structural defects particularly prevalent in highly siliceous zeolites. This work demonstrates a different approach that synergistically integrates zeolite acidity and defect engineering. A hydrothermal synthesis strategy with a selected inorganic source precisely controls aluminum incorporation into the highly siliceous CHA zeolite framework (Si/Al > 800). Subsequently, a postsynthetic fluorination followed by calcination effectively heals silanol defects. The resulting HS-CHA-F zeolite features a hydrophobic framework that facilitates rapid methanol diffusion while utilizing precisely tuned ultraweak acidity to steer selective C–C coupling. The optimized OXZEO bifunctional catalyst ZnZrOx/HS-CHA-F achieves 38.5% CO2 conversion and 91.3% light olefin selectivity in hydrocarbons at 653 K and 4 MPa, substantially outperforming conventional SSZ-13 and SAPO-34 benchmarks. This study establishes a generalizable method for overcoming long-standing limitations in CO2 hydrogenation through coupled zeolite acidity and defect engineering.
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ChemCatChem
·
2026
·Vol. 18
·期 2
·e01534
·
IF 3.9
Wenbin Huang,Haoran Liu,Han Yang,Zhen Xu,Tianyu Bai,Fan Shao,Yasong Zhou,Qiang Wei
To improve the efficiency of existing Cu-layered double oxide (LDO) catalysts for hydrogenation of CO 2 to methanol, graphene oxide (GO)-doped Cu-LDO/xGO catalysts were successfully prepared by coprecipitation method, and the influence of GO doping on the structure and reaction performance of Cu-LDO catalysts was deeply investigated. Characterizations including XRD, SEM, ICP-OES, N 2 physical adsorption-desorption, TEM, N 2 O chemisorption, H 2 -TPR, and H 2 /CO 2 -TPD reveal that optimal GO loading (2 wt%) promoted the formation of highly dispersed Cu particles and abundant Cu─MgO interfaces, enhancing H 2 adsorption/dissociation and CO 2 activation. The Cu-LDO/2.0GO catalyst achieved a CO 2 conversion of 22.4%, CH 3 OH selectivity of 94.5%, and methanol space-time yield (STY) of 652.1 g·kgcat −1 ·h −1 at 240°C and 2.5 MPa-outperforming the GO-free Cu-LDO/0GO catalyst, and long-term stability tests show that the incorporation of GO mitigated Cu sintering, maintaining catalytic activity over 200 h. The results of structure-activity relationship analysis show that the main reason 2 wt% GO doping significantly improved the activity and stability of the catalyst lies in the synergistic effect: GO improved Cu sites dispersion boosting H 2 activation and Cu─MgO interface formation. Meanwhile, GO can also act as a conductive bridge for H spillover, enabling hydrogenation of formate and other intermediates adsorbed on Cu–MgO interfaces that are not in direct contact with conventional Cu surfaces, potentially involving isolated Cu species. The study establishes that rational GO incorporation optimizes active site utilization, providing a strategy for designing efficient catalysts for CO 2 conversion. Graphical The incorporation of GO enhances the dispersion of the active metal Cu and increases the density of surface base sites in the catalyst, thereby accelerating the rate of methanol production via CO 2 hydrogenation.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Laigang Hu,Weiwei Wang,Ling Jiang,Jinru Hu,Hongxia Zhu,Mengxue Zhang,Jian Wu,Daohui Lin,Kun Yang
Exploring CO 2 adsorption under humid conditions is crucial for practical applications. Herein, ZJU-521(Al) was synthesized using low-toxicity helical secondary building units (SBUs, [Al 5 (OH) 7 (−COO) 8 ] ∞ ) and tetrakis (4-carboxyphenyl)methane (H 4 MTTB) ligand, with excellent chemical stability. Saturated CO 2 adsorption capacities of ZJU-521(Al) reach 6.19 mmol/g at 273 K and 4.52 mmol/g at 298 K, respectively, and moderate isosteric heat of 28.23 kJ/mol, enabling low-energy regeneration. Simulation results reveal two CO 2 adsorption sites on ZJU-521(Al): site I, located near the helical SBUs and interwoven with the helical SBUs, and site II, situated near the H 4 MTTB ligand. ZJU-521(Al) can effectively separate CO 2 from the CO 2 /N 2 mixture, as identified by the ideal adsorbed solution theory values of 28.81 at 273 K and 40.83 at 298 K for CO 2 /N 2 (15/85) mixture, respectively. Dynamic adsorption experiments reveal dynamic CO 2 adsorption of 0.59 mmol/g under dry conditions and 0.54 mmol/g at 80% relative humidity (RH) for ZJU-521(Al), highlighting its moisture-resistant behavior for CO 2 adsorption under humid conditions. Most adsorbed CO 2 is readily desorbed by argon purging at 14 min (dry) and 12 min (80% RH) at 298 K, respectively. Therefore, ZJU-521(Al) emerges as a promising candidate for efficient CO 2 adsorption, separation, and desorption even under humid conditions.
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Nature Communications
·
2026
·
IF 15.7
Shi Yingli,Liu Ying,Dong Hongchun,Fu Gaocheng,Zhou Hang,Wang Haifeng,Wang Xue-Lu,Yao Ye-Feng
The proton-coupled electron transfer (PCET) kinetics plays a critical role in governing the CO 2 -to-formate conversion efficiency during CO 2 eletroreduction reaction. While alkali metal cations are known to influence the reaction pathway, elucidating how trace doping modifies the catalytic sites remains a key challenge. Here we show that incorporating Li into bismuth oxycarbonate (BOC-Li) induces structural modifications that optimize the PCET process at bismuth-active sites, thereby boosting CO 2 -to-formate conversion. By employing dual-isotope ( 2 H/ 13 C) operando nuclear magnetic resonance (NMR) to track the formation of 1 H 13 COO − / 2 H 13 COO − , combined with kinetic isotope effect, Tafel analysis and in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy, we observe a more efficient proton-electron transfer pathway. Density functional theory (DFT) calculations suggest that Li doping is associated with enhanced activity of Bi sites, potentially strengthening H 2 O/CO 2 adsorption and reducing the O–H activation energy. Collectively, this work highlights alkali doping as a promising strategy for structurally engineering catalytic sites to improve PCET kinetics.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9
Heyang Dou,Yajun Li,Dayang Wang,Qian Zhu,Dewen Hou,Jian Qi
In the field of photocatalytic conversion, the efficiency of charge separation between photogenerated electrons and holes is a critical determinant of catalytic performance. However, the development of highly efficient photocatalysts and the precise modulation of their electronic orbitals remain significant challenges. In this study, PbTiO 3 powder was first successfully synthesized via the high-temperature solid-state method. Subsequently, surface oxygen vacancies were introduced through a hydrothermal acid-induced treatment. Experimental results demonstrate that the PbTiO 3 sample with the highest concentration of oxygen vacancies exhibits significantly enhanced photocatalytic performance, achieving a 19-fold increase in activity compared to pristine PbTiO 3 . The CO evolution rate reaches 16.26 μmol·g −1 ·h −1 , with a selectivity of 92.71%. A comprehensive investigation into the underlying mechanism reveals three key contributing factors. First, the abundant formation of oxygen vacancies provides a high density of active sites for CO 2 adsorption and activation, thereby promoting the catalytic reaction; Second, the reduced band gap width facilitates the generation of photogenerated electron-hole pairs by lowering the energy threshold for electronic transitions, thereby improving charge carrier generation and electron transport efficiency. Third, in PbTiO 3 , electrons are transferred from titanium to oxygen atoms, accompanied by electron filling from the t 2g to the e g orbitals of oxygen. This results in increased electron density in the e g orbitals, which enhances the capacity of oxygen vacancies to capture electrons. Therefore, the modulation of the electronic state significantly enhances the separation efficiency of photogenerated electron-hole pairs. Based on the aforementioned optimization strategies, this study offers novel insights and methodologies for the design of efficient photocatalytic systems with orbital regulation capabilities, and holds promise for advancing the broader application and development of photocatalytic technologies in areas such as energy conversion and environmental remediation.
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JOURNAL OF MATERIALS CHEMISTRY
·
2012
·Vol. 22
·期 43
·23136-23140
·
IF 5.968
Yong Cui,Ruiping Deng,Gang Wang,Daocheng Pan
Quaternary semiconductor Cu2MSnS4 (M = Co2+, Fe2+, Ni2+, Mn2+) nanocrystals have been successfully synthesized via a simple and mild solvothermal method. Cu2FeSnS4 and Cu2CoSnS4 show a spherical shape; Cu2NiSnS4 and Cu2MnSnS4 possess a nail-like structure and a rod-like structure. The four types of nanocrystals exhibit significantly different magnetic properties. Cu2FeSnS4 and Cu2CoSnS4 nanoparticles show ferromagnetic behavior; Cu2MnSnS4 and Cu2NiSnS4 nanorods exhibit superparamagnetic behavior at low temperature. The band gaps of Cu2MSnS4 (M = Co, Fe, Ni, Mn) nanocrystals are in the range of 1.2–1.5 eV, indicating a high potential application in low-cost thin film solar cells.
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REACTIVE & FUNCTIONAL POLYMERS
·
2022
·
IF 4.966
Chenjie Li,Yulin Ding,Wei Xu,Minyu Li,Wenmu Li
Introducing CO 2 affinity additives into membrane is one of significant approaches to improve the CO 2 permeability of membranes for natural gas sweetening. In current work, high performance mixed-matrix membranes were successfully obtained using the cellulose acetate (CA) and the zeolitic tetrazolate-imidazolate frameworks (ZTIFs) with highly CO 2 affinity as matrix and additive respectively. The interaction between CA matrix and ZTIFs was verified by the FT-IR. The SEM, EDS and XRD were used to evaluate the morphology properties of these membranes. The CO 2 permeability of CA/ZTIFs mixed-matrix membranes which is closely correlated to the loading of high CO 2 affinity ZTIF additive were in a range of 9.59–15.85 Barrer, implying the indispensable role of the ZTIF additive in changing the CO 2 dissolution and diffusion behavior inside the membranes. The ideal compatibility and gas selectivity proved the great potential of the ZTIFs additives for the gas separation application.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Yu Kang,Yujia Han,Cong Wei,Kuo Liu,Ming Tian,Chuande Huang,Chaojie Wang,Jian Lin,Baolin Hou,Xiaoli Pan,Yang Su,Lin Li,Riguang Zhang,Yong Hao,Xiaodong Wang
Thermochemical two-step CO 2 splitting is a potential approach that fixes the sustainable resource into transportable liquid fuels. However, the harsh CO 2 splitting conditions, the limited oxygen release kinetics and capacity of metal oxides block further promoted the CO yield and solar-to-fuel energy efficiency. Here, we propose a different carbon cycle assisted by Ni/La 2 O 3 via coupling methane decomposition with thermochemical CO 2 splitting, replacing conventional metal oxides cycle. Superior performance was demonstrated with methane conversion reached around 94% with almost pure H 2 generation. Encouragingly, CO 2 conversion of 98% and CO yield of 6.9 mmol g −1 derived from CO 2 were achieved, with peak CO evolution rate (402 mL min −1 g −1 ) of orders of magnitude higher than that in metal oxide process and outstanding thermodynamic solar-to-fuel energy efficiency (55.5% vs. 18.5%). This was relevant to the synergistic activation of La 2 O 3 and Ni for CO 2 in carbon cycle, thus improving CO 2 splitting reaction with carbon species.
研究领域:
能源化学
·
催化化学
·
可持续能源
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热化学转化
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二氧化碳利用
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高影响因子
JOURNAL OF MATERIALS CHEMISTRY
·
2011
·Vol. 21
·期 40
·16028-16034
·
IF 5.101
Jun Shi,Zhengzheng Zhang,Gefei Li,Shaokui Cao
Alginate/CaCO3 hybrid beads with pH- and thermal-responsive drug release properties were prepared under compressed CO2 using aliphatic poly(urethane-amine)s (PU) as the thermal-responsive component. Polyacrylic acid (PAA) was used as a crystal growth additive to control the structure of the hybrid beads. The hybrid beads were characterized by using scanning electron microscopy, X-ray powder diffraction and thermogravimetric analysis. The interaction between PAA and aliphatic PU contributed to the formation of alginate beads with a compact CaCO3 shell. Indomethacin release behaviour was found to be pH- and thermal-responsive. The release profiles were sustained with CaCO3 microparticles, indicating that the compact CaCO3 shell could hinder the permeability of the encapsulated drug and reduce the drug release effectively. The results suggest that the hybrid alginate beads can be used as “smart” polysaccharide materials for sustained dual-responsive drug delivery.
研究领域:
生物材料
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药物递送系统
·
高分子科学
·
纳米医学
·
药剂学
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生物化学
·
组织工程
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高影响因子
Journal of Materials Chemistry A
·
2026
·
IF 9.5
Yongshu Wang,Yujia Han,Zuwei Luo,Xiaohui Hu,Wendian Shi,Minghao Ma,Yuxiang Shen,Houfu Lv,Guoxiong Wang,Xinhe Bao
Metal exsolution in perovskite oxide has emerged as an effective way to boost CO2 electrolysis activity in solid oxide electrolysis cells (SOECs). It is crucial to precisely tailor the exsolution characteristics to optimize the catalytic functionality and boost the catalytic activity. Herein, we reveal that the Cr cations doping effectively modify the crystal defects and regulate the metal exsolution of Sr2Fe1.1Ni0.2Cr0.2Mo0.5O6-δ (SFNCM). FeNi alloy nanoparticles with an average particle size of ~10 nm and a particle density of exceeding 1500 μm-2 were exsolved on the surface of SFNCM perovskite, which increases the active sites and enhances CO2 electrolytic activity. The SFNCM based SOEC decorated with abundant FeNi alloy nanoparticles achieves a high current density of 2.57 A cm-2 at 1.6 V, superior to other Sr2Fe1.3Ni0.2Mo0.5O6-δ counterparts.The experimental and theoretical calculation results demonstrate the controllability of the exsolution via engineering of the perovskite structural feature. This work offers a new perspective on lattice doping strategy for the regulation of metal exsolution.
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CHINESE JOURNAL OF CATALYSIS
·
2026
·
IF 17.7
Juxia Xiong,Hao Ma,Yingjun Dong,Benjamin Liu,Xiangji Zhou,Linbo Li,Yuanmiao Sun,Xiaolong Zhang,Hui-Ming Cheng
Bi-based catalysts are known to promote the electrochemical reduction of CO 2 to formic acid (HCOOH) or formate (HCOO − ). However, their implementation presents challenges: the first H + /e − pair transfer to form the key *OCHO intermediate on a Bi surface is a slow, kinetically sluggish endergonic process, resulting in a large overpotential and narrow potential window for high HCOOH/HCOO − selectivity. Altering the localized p -orbital electron states of Bi to change intermediate binding behaviors is difficult. We addressed this problem by using an in-situ polymerization method to obtain a polyaniline-Bi hybrid (PANI-Bi) with Bi surrounded by PANI chains. Combined experimental and computational studies indicate that the polyaniline acted as an “electron pump” that facilitated charge transfer from the PANI backbone to the Bi surface and changed the p -orbital electrons of the Bi active sites. This lowered the energy barrier for the adsorption of intermediates and facilitated *OCHO formation. Consequently, a significant increase in formate production was observed, achieving a single-pass carbon efficiency exceeding 48.7% at 800 mA cm −2 . This organic functionalization strategy, aimed at modifying the electronic structure of heterogeneous catalysts, offers a promising approach for achieving highly selective electroreduction of CO 2 at a high current density.
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