SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Qiang Zheng,Zhenguo Liang,Derui Li,Fuxin Yang,Houzhang Tan,Xiaopo Wang
Deep eutectic solvent (DES) has the potential to replace aqueous amines for carbon capture. However, the reported DESs fail to absorb CO 2 equivalent to that absorbed by aqueous amines. To combine the excellent performance of amines and DESs, 9 amine-based DESs were prepared. The tetraethylammonium chloride was selected as the hydrogen bond acceptor, while ethanolamine, diethanol amine and triethanolamine were selected as the hydrogen bond donors. The molar ratios range from 1:4 to 1:6. Their properties were analyzed, including the structure, the thermal behavior and the potential corrosion. It has been determined that all DESs show a large liquid range (200 ∼ 600 K). Furthermore, the absorption characteristics of 9 DESs were studied. It has been found that the absorption capacity of DES3 and DES5 can reach up to 0.4066 and 0.3752 mol CO 2 /mol absorbent respectively, even 3 ∼ 6 times amount compared with the corresponding aqueous amines. At the laboratory level, the heat duty for the desorption process at 413.15 K of DES1 is 21.31 % of that for that of 30 wt% MEA at 393.15 K. For DES5, this value is 6.70 %. Besides, these DESs can maintain their splendid performance in absorption–desorption after 5 cycles. Meanwhile, the thermal stability and viscosity of the rich-absorbents were analyzed. Rich-absorbents are stable. Furthermore, effects of water have been inspected. The added water reduces the viscosity but confines the absorption capacity. For balance, the addition of 10 wt% water is recommended. Finally, the absorption mechanism was revealed. Both the physical and chemical absorption promote the absorption capacity of DESs.
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高影响因子
ACS Applied Nano Materials
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2025
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IF 5.5
Yilin Wang,Yuping Chen,Shuang Yao,Furong Zhao,Linxiu Dai,Xian Yang,Changhua An
Electrochemical CO2 energization represents a promising strategy to mitigate its emission and promote resourceful utilization. The production of alcohols offers a sustainable pathway for converting CO2 into value-added chemicals, which is often hindered by low selectivity and high overpotential. In this work, a class of ultrasmall La2O3 nanoparticle-modified Cu2O-based catalyst has been synthesized in situ on a copper foam substrate through a simple hydrothermal method. The optimized catalyst demonstrated a high ethanol Faradaic efficiency of 51.7% at −1.0 V versus the reversible hydrogen electrode (RHE); simultaneously, syngas (CO/H2) was generated with Faradaic efficiencies of 28.27% for CO and 4.8% for H2. This product distribution characteristic enables efficient separation and utilization of both liquid (ethanol) and gaseous (syngas) products. This study highlights the pivotal role of rare earth elements in enhancing CO2RR efficiency by stabilizing reaction intermediates for facilitating C–C coupling. Furthermore, it presents a scalable and cost-effective approach for CO2 energization, paving the way for sustainable green energy production and carbon resource management.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Xueli Zhou,Qingyuan Song,Jing Chen,Chunhong Chen,Yuhuan Chen,Fang Yang
Blended amine mixtures show great superiorities in CO 2 absorption capacity and energy efficiency. This work focuses on the absorption-desorption performance of CO 2 capture by mixed amine solutions based on N, N-diethylethanolamine (DEEA). Four bi-solvent blends consisting of DEEA and 2-amino-2-methyl-1-propanol (AMP)/1-(2-hydroxyethyl) piperazine (HEPZ)/1-ethylpiperazine (N-1EPZ)/piperazine (PZ) are studied. The CO 2 loading, absorption rate, average absorption rate, desorption loading, average desorption rate, desorption efficiency and relative heat duty are comprehensively investigated to explore the performance of blended absorbents. Experimental investigations on concentration reveal that blended 20 wt% DEEA +10 wt% PZ solution demonstrates outstanding CO 2 equilibrium loading, absorption rate and average absorption rate, and 20 wt% DEEA +10 wt% AMP system exhibits excellent CO 2 desorption performance. The average desorption rate, desorption loading and desorption efficiency increase by 91.47 %, 91.09 % and 122.30 % in contrast to the single amine solution, i.e. aqueous 30 wt% MEA, respectively. Therefore, mixed amine solutions can largely reduce the energy requirement for CO 2 regeneration, which confirms blended amine mixtures are energy-efficient. Additionally, 13 C NMR and FT-IR spectra are conducted to elucidate the mechanism of DEEA-based mixed amine systems for CO 2 capture.
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ADVANCED MATERIALS
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2025
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IF 26.8
Yuchun Liu,Tianqi Liu,Xinyun Wang,Jing Zhang,Xingwu Zhai,Tianchen Wei,Qianqi Shi,Chengjie Lu,Huan Yan,Yujian Xia,Weiren Cheng,Min Zhou
Li-CO₂ batteries promise ultrahigh theoretical energy densities but face efficiency limitations owing to the sluggish decomposition of stable Li 2 CO 3 . Redirecting the redox pathway toward Li 2 C 2 O 4 overcomes this challenge, but its metastability leads to facile conversion to Li 2 CO 3 during discharge. Herein, subsurface electronic confinement is engineered in Mo-based catalysts, leveraging electron-deficient boron (B) as electron traps in the subsurface atomic layers to tailor their interfacial electronic landscapes. This design elevates the Mo d-band and intensifies the hybridization between the Mo d-orbitals and O p-orbitals of oxalate. Strengthening the Mo-O interaction stabilizes Li 2 C 2 O 4 against decomposition. The highly reversible and stable redox chemistry enabled by MoB results in an exceptional cycling stability and energy efficiency across a wide temperature range, with an expanded practical viability. At 70 µA cm −2 , the MoB-based battery is cycled for >1400 h with a high energy efficiency of >85%. The energy efficiency even remains at >90% for ≈150 h at a high temperature (90 °C). This study pioneers a material design framework for use in stabilizing metastable products within Li-CO 2 batteries, advancing their applicabilities in extreme environments, such as deep-earth exploration, by revealing the role of subsurface charge redistribution in steering reaction pathways.
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PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Xiarui Yan,Junsheng Chen,Zhaorui Kong,Xinyi Wan,Youmin Hou,Bin Hua
Research on CO2 hydrogenation catalysts, particularly In2O3-based materials, is crucial for developing sustainable CO2 utilization and chemical production technologies, contributing to a cleaner future. We address the critical challenge of efficient and stable CO2 conversion by developing a novel Zr-doping strategy to enhance In2O3 catalyst performance for CO2 hydrogenation to methanol. Our key contribution is identifying the nanoscale confinement effect as crucial for optimizing both the activity and stability of In2O3 catalysts. By leveraging this nanoscale confinement effect, we have precisely controlled the size, dispersion, and reducibility of In2O3 nanoparticles, resulting in the formation and stabilization of highly active In2O3–x with oxygen vacancies. This confinement also effectively suppresses In0 migration and sintering, dramatically improving catalyst stability. The resulting Zr-doped catalysts exhibit significantly higher activity and stability compared to the undoped In2O3/ZrO2 catalyst, achieving a remarkable space-time yield of 4.708 gMeOH gIn–1 h–1 and demonstrating durability under industrially relevant conditions. This discovery offers a promising new direction for the rational design of high-performance CO2 hydrogenation catalysts and lays the foundation for future advances in sustainable catalysis.
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ACTA PHYSICO-CHIMICA SINICA
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2025
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IF 13.5
Qinhui Guan,Yuhao Guo,Na Li,Jing Li,Tingjiang Yan
In the realm of photocatalytic CO 2 hydrogenation, the adsorption-desorption behaviors and dynamics of photogenerated carriers are pivotal determinants of the kinetic processes and overall efficiency of photocatalytic reactions. Herein, 5A molecular sieve-functionalized In 2 O 3 composites (denoted as IO@5A- x wt%) were fabricated through a facile impregnation-calcination method. Among them, the IO@5A-5wt% composite, with the optimized loading amount of 5A molecular sieves, showcases outstanding performance in photocatalytic conversion of CO 2 to CO, achieving a CO production rate of 2610.55 μmol·g −1 ·h −1 , which is 19 times higher than that of pristine In 2 O 3 . Moreover, the IO@5A-5wt% composite maintains acceptable catalytic stability after a prolonged experiment lasting 45 hours and total of 108 cycles. A comprehensive series of characterization techniques and performance evaluations reveal that the incorporation of 5A molecular sieves significantly modulates the adsorption-desorption behavior and hole dynamics during photocatalytic reactions. The multi-channel architecture of 5A molecular sieves, featuring suitable pore sizes, effectively enhances CO 2 adsorption. Meanwhile, the surface hydroxyl groups of 5A molecular sieves facilitate the transfer of photogenerated holes, thereby suppressing the recombination of photogenerated carriers. Additionally, the reaction product H 2 O desorbs more readily from the catalyst surface. These synergistic effects collectively constitute the key mechanism underlying the enhanced photocatalytic performance of the IO@5A-5wt% composite.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Xiaopeng Li,Haichao Wang,Qingxiang Ma,Jucang Ke,Xiuyun Jiang,Caixia Zhu,Linlin Zhao,Ao Zhang,Hao Chen,Yao Deng,Xinhua Gao,Guangbo Liu,Tian-Sheng Zhao,Noritatsu Tsubaki
The conversion of CO 2 into ethanol with value-added still exists challenge, especially the CO 2 hydrogenation over Co-based catalysts is still C1 product dominated by CH 4 . Here, we report a xNa-CoMnO catalyst to promoting ethanol synthesis from CO 2 hydrogenation. The experimental results indicated that there was almost no adsorption and conversion of CO 2 on pure Co 0 , and the CO 2 hydrogenation production of the CoMnO catalyst prepared by adding Mn was mainly CH 4 . The loading of Na not only increased the concentration of oxygen defects on the CoMnO catalyst, but also improved the strength of the Co-O in the CoMnO catalyst, which was able to adsorb effectively the undissociated *CO in the reaction process, and promote the C-C coupling between the *CO and the generated *CH x , promoted the synthesis of ethanol. Under optimized reaction conditions (240 °C, 3.0 MPa, GHSV = 1200 mL/g/h), the 2Na-CoMnO catalyst showed ethanol selectivity of 18.89 % and space-time yield of ethanol of 1.27 mmol/g/h, which exceeded most of the reported results. More importantly, beyond delivering an excellent-performance catalytic system, this study also provides fundamental insights for the rational design of Co-based catalysts for selective CO 2 -to-ethanol conversion.
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ACS Nano
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2022
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IF 18.027
Peng Wang,Tan Li,Qiqi Wu,Ruian Du,Qinghua Zhang,Wei-Hsiang Huang,Chi-Liang Chen,Yan Fan,Haonan Chen,Yanyan Jia,Sheng Dai,Yongcai Qiu,Keyou Yan,Yuanyuan Meng,Geoffrey I. N. Waterhouse,Lin Gu,Yun Zhao,Wei-Wei Zhao,Guangxu Chen
In certain metalloenzymes, multimetal centers with appropriate primary/secondary coordination environments allow carbon–carbon coupling reactions to occur efficiently and with high selectivity. This same function is seldom realized in molecular electrocatalysts. Herein we synthesized rod-shaped nanocatalysts with multiple copper centers through the molecular assembly of a triphenylphosphine copper complex (CuPPh). The assembled molecular CuPPh catalyst demonstrated excellent electrochemical CO2 fixation performance in aqueous solution, yielding high-value C2+ hydrocarbons (ethene) and oxygenates (ethanol) as the main products. Using density functional theory (DFT) calculations, in situ X-ray absorption spectroscopy (XAS) and quasi-in situ X-ray photoelectron spectroscopy (XPS), and reaction intermediate capture, we established that the excellent catalytic performance originated from the large number of double copper centers in the rod-shaped assemblies. Cu–Cu distances in the absence of CO2 were as long as 7.9 Å, decreasing substantially after binding CO2 molecules indicating dynamic and cooperative function. The double copper centers were shown to promote carbon–carbon coupling via a CO2 transfer-coupling mechanism involving an oxalate (OOC–COO) intermediate, allowing the efficient production of C2+ products. The assembled CuPPh nanorods showed high activity, excellent stability, and a high Faradaic efficiency (FE) to C2+ products (65.4%), with performance comparable to state-of-the-art copper oxide-based catalysts. To our knowledge, our findings demonstrate that harnessing metalloenzyme-like properties in molecularly assembled catalysts can greatly improve the selectivity of CO2RR, promoting the rational design of improved CO2 reduction catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Ning Zhang,Yingmei Meng,Zhiying Li,Chuanlong Jin,Junjiang Bao,Xiaopeng Zhang,Gaohong He
High free-volume microporous membranes constructed by intrinsically microporous polymers (PIMs) are up-and-coming in efficient carbon capture, but their practical applications are limited by plasticization and physical aging issues. This work we proposed a CO 2 -solution-compensated cross-linking strategy to construct microporous membranes with both crosslinking network and enhanced CO 2 solubility via the Hoffmann alkylation reaction between the bromomethylated PIM matrix and Ethylenediamine (EDA) only at 80 °C. The enhanced CO 2 solubility could compensate the reduced CO 2 diffusion by the crosslinking network. Accordingly, the crosslinked microporous membranes with CO 2 -solubility compensation achieved a superior decarbonization from natrual gas (CO 2 permeability of 898.9 Barrer, CO 2 /CH 4 separation factors of 204.1) surpassing the 2019 Robeson upper and excellent anti-plasticization (plasticizing pressure up to 0.8 MPa) and anti-aging (CO 2 permeability loss < 10 % after 30 days) performance. The CO 2 -solubility-compensation crosslinking strategy will promote the development of high-performance microporous membrane for efficient decarbonization.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Bei Liu,Mingxing Zhou,Zhinan Wu,Xulong Song,Tong Zhou,Shipeng Cao,Chongjian Jiang,Xinwei Zhang,Xiwen Zhang,Liwen Mu,Han Lin,Xiaohua Lu,Tuo Ji,Shuandi Hou,Jiahua Zhu
Amine-based sorbents are promising for low-concentration CO 2 capture, yet their practical application has long been hindered by poor stability. In this study, amidated tetraethylenepentamine (TEPA) network (ATN) sorbents were synthesized by crosslinking TEPA with 4 binary organic acids in the molded alumina-silica (MAS) supports. Characterizations confirm the successful formation of amide bonds between the primary amines of TEPA and binary acids within the pore channels, a key innovation that reconfigures TEPA distribution—shifting from a wall-attached state (as in conventional systems) to an aggregated polymeric network. This structural breakthrough yields remarkable stability enhancements: unlike TEPA/MAS, which loses ∼90 % of its initial capacity after 50 cycles, TEPA/MAS- t , t -MA, and TEPA/MAS-FA retain ∼80 % of their capacity under the same conditions. Experimental results and DFT calculations further reveal a novel mechanistic insight: acids containing double bonds form more stable amide networks with stronger p-π conjugation than straight-chain acids. By integrating molecular crosslinking with porous support engineering, this strategy offers a robust framework for designing durable, high-performance CO 2 capture materials for actual applications.
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高影响因子
Science China-Chemistry
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2025
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IF 9.7
Li Ran,Yin Hang,Jing Wen-Kai,Cheng Jia-Lin,Qin Xue-Rong,Lu Tong-Bu,Wang Hong-Juan,Yu Zi-You
As important catalysts for C–C coupling, copper-based materials have great potential for electrocatalytic reduction of CO 2 to C 2+ products. In this work, Cu 2 O catalysts modified with different lanthanide hydroxides were successfully synthesized and used for CO 2 electroreduction. The results showed that compared with Cu 2 O/Gd(OH) 3 and Cu 2 O/Yb(OH) 3 catalysts, Cu 2 O/La(OH) 3 exhibited the highest electrocatalytic performance for CO 2 reduction. This catalyst was able to maintain a high Faraday efficiency for C 2+ products ( \({\rm FE}_{{\rm C}_{2+}}\) ) of about 60% within the current density range of 400–800 mA cm −2 . The highest \({\rm FE}_{{\rm C}_{2+}}\) reached 66% at 600 mA cm −2 and the partial current density for C 2+ products reached a maximum of 488 mA cm −2 . Meanwhile, the catalyst could run stably for 40 h with a remained \({\rm FE}_{{\rm C}_{2+}}\) of about 60%. Multiple characterizations reveal that the introduction of La(OH) 3 promotes the formation of *CO intermediates, and also helps to stabilize the Cu(I) species in Cu 2 O under cathodic potentials, thus facilitating the C–C coupling for C 2+ production. This work provides a new strategy to enhance the C 2+ production via stabilizing Cu(I).
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高影响因子
SOLID STATE SCIENCES
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2025
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IF 3.3
Feng-Jun Zhang,Zi-Chen Wang,Yu-Hong Niu,Jie Ma
For ultimate photocatalytic CO 2 reduction efficiency, In 2 O 3 synthesized via co-precipitation/calcination was architecturally integrated with Bi 2 MoO 6 through solvothermal assembly, constructing composite catalysts. In 2 O 3 incorporation triggered absorption edge red-shifting, quenched photoluminescence, and amplified photocurrent density. The 2 %-In 2 O 3 composite delivered 12.5 μmol/g/h CO yield under 300W xenon lamp – achieving a 2.5-fold enhancement versus pure In 2 O 3 and a 1.8-fold gain relative to pure Bi 2 MoO 6 . This superiority arose from heterostructuring induced by In 2 O 3 loading, which expedited photogenerated carrier mobility and elevated CO 2 conversion activity.
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