CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Xing Yan,Dongren Cai,Meihong Lin,Zhijie Wu,Yegang Xia,Yanmei Cai,Sajid Ali,Kok Bing Tan,Andriambinintsoa Ranaivoson Tojonirina,Hao Sun,Guowu Zhan
The selective hydrogenation of CO 2 to methanol demands precise control of both catalyst architecture and reaction pathways. Here, we design an atomic layer deposition (ALD)-engineered Pd/ZnO/ZrO 2 ternary catalyst with atomic-scale ZnO interlayers to decouple and reconfigure active sites at dual interfaces (Pd-ZnO and ZnO-ZrO 2 ). This interfacial engineering drives a 7-fold enhancement in methanol space–time yield (0.584 vs. 0.084 g MeOH g cat −1 h −1 ) and switches the dominant reaction pathway from CO-mediated to formate-driven selectivity (methanol selectivity remarkably surges from 6 % to 64 %). Multimodal characterization and theoretical calculations reveal that ZnO interlayers orchestrate bifunctional cooperation: activating CO 2 /CO adsorption while suppressing CO/CH 4 formation through electronic effects. Long-term stability study uncovers a dynamic restructuring mechanism, where Pd-ZnO interfaces gradually evolve into PdZn β alloy phases under the reaction conditions. This work establishes ALD-mediated interface design as a generalizable strategy to manipulate reaction networks and methanol selectivity in catalytic CO 2 hydrogenation systems.
研究领域:
催化化学
·
材料科学
·
化学工程
·
可持续能源
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表面科学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2025
·
IF 4.5
Shuang Wang,Dudu Li,Zelong Xu,Fan Zhou,Zhihua Qiao,Zibo Yang,Zhi Wang
Coordination polymer (CP) glasses offer high processability and permanent accessible pores, having promising potential in gas separation. However, their low porosity makes it difficult to prepare high-performance gas separation membranes. In this work, we combined the advantages of CP glasses and inorganic fillers, and selected ag Zn-P-dmbIm as the continuous phase and hydroxylated multi-walled carbon nanotubes (HMWCNTs) as the dispersed phase to prepare HMWCNTs/ ag Zn-P-dmbIm mixed matrix membranes (MMMs). The very favorable interfacial compatibility and excellent CO 2 /N 2 gas separation performance of the MMM-2 membrane were demonstrated by a series of characterizations. The test results revealed that the CO 2 permeability and ideal CO 2 /N 2 selectivity of MMM-2 membrane were 9776.8 Barrer and 31.1, respectively, which exceeded the Robeson 2019 upper bound. In addition, the well-defined long-term stability of the MMM-2 membrane lays the foundation for realizing gas separation membranes for industrial applications in practice. This provides a strategy for the subsequent preparation of CP glasses-based MMMs.
研究领域:
材料科学
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膜技术
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气体分离
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高分子化学
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纳米复合材料
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Zhihao Song,Xinrui Liu,De Ao,Zhihua Qiao,Zhi Wang,Song Zhao
Metal-organic framework glass shows great promise in gas separation applications, however, its inherent low porosity poses significant challenges to achieve the enhanced membrane permeability. In this work, we developed novel self-standing crystal-glass composite membrane via melt quenching process of porous organic cages and coordination polymer glasses. The resulting (CC3) n /( a g Zn-P-dmbIm) 1-n membranes effectively combines the high porosity of CC3 with the excellent film-forming property of Zn–P-dmbIm glass, enabling efficient CO 2 /CH 4 separation. Specifically, CO 2 molecules are preferentially adsorbed into the CC3 channels, followed by rapid permeation through the membrane, while the size exclusion restricts CH 4 molecules transport through the membranes. The obtained (CC3) 0.05 /( a g Zn-P-dmbIm) 0.95 membrane achieves a high CO 2 permeability of 9358 Barrer, a CO 2 /CH 4 selectivity of 24.2, and demonstrates 24-h operational stability. This study not only broadens the application scope of coordination polymer glasses in gas separation membranes but also provides novel insights for the design of high-performance crystal-glass composite membranes.
研究领域:
材料科学
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膜技术
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气体分离
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可持续能源
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聚合物化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Chaogang Ban,Yang Wang,Jiangping Ma,Yajie Feng,Junjie Ding,Youyu Duan,Xue Liu,Bin Zhang,Jinjing Tang,Xiaoping Tao,Liyong Gan,Shuangshuang Tan,Xiaoyuan Zhou
Rational fabricating advanced photocatalysts to recycle CO 2 into solar fuel is one of the most promising approaches to simultaneously address energy shortages and global warming. TiO 2 has been widely used in photocatalytic CO 2 reduction due to its abundant reserves, non-toxicity and harmlessness etc. However, it remains significantly challenging for practical applications due to the fast electron-hole recombination. Herein, we design a direct TiO 2 based Z-Scheme heterojunction by self-assembly of C-doped TiO 2 nanoparticles on 3D hierarchical petal of flower-like β-Bi 2 O 3 (C-TiO 2 /β-Bi 2 O 3 ). In situ electron paramagnetic resonance tests, in situ X-ray photoelectron spectroscopy and theoretical calculations reveal that electrons are transferred from β-Bi 2 O 3 to C-TiO 2 due to the formation of Z-Scheme heterojunction, which greatly accelerates the separation of photogenerated carriers to promote efficient CO 2 photoreduction. Ultimately, the optimal heterojunction shows significantly enhanced photocatalytic activity for CO 2 reduction to CO (31.07 μmol g –1 h −1 ) compared to the pure TiO 2 (3.28 μmol g –1 h −1 ) without using any photosensitizers and sacrificial agents. This work provides a unique insight to design direct Z-Scheme heterojunctions and delivers a promising photocatalyst for overcoming global warming and energy-supply issues.
研究领域:
材料科学
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环境科学
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化学工程
·
光催化
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Ningbo Yu,Qiang Sun,Minghao Wang,Huiying Liao,Zhiwu Liang,Hongxia Gao
Water-lean absorbents have garnered significant attention for CO 2 capture due to their advantages of low corrosivity and reduced regeneration energy consumption. However, current research indicates that alcohol-based solvents generally exhibit inhibiting effects on CO 2 absorption kinetics, and the underlying suppression mechanisms remain unclear. This study employs molecular dynamics simulations to confirm that the kinetic inhibition mechanism induced by alcohols stems from dual regulatory effects where alcohol molecules form a tighter solvation shell around amines to impede zwitterion formation, while their hydrophobic alkyl groups disrupt hydrogen-bond networks to hinder zwitterion deprotonation. Further research reveals a significant structure-kinetic relationship in 3AP-alcohol solutions, where increased chain length and branching degree of alcohols correlate with slower reaction kinetics. Through integrated analysis of electrostatic potential, non-covalent interactions (NCI), and charge density, we elucidate how solvent effects inhibit the 3AP-CO 2 reaction by three mechanisms: reducing the negative electrostatic potential contribution at the amino nitrogen site, increasing transition-state bonding resistance, and decreasing charge transfer efficiency. The validity of this structure-kinetic mechanism was confirmed by our established kinetic model (AARD <4 %). This study provides a theoretical basis for the solvent screening of CO 2 poor water absorbents, which is helpful for the development process of absorbents.
研究领域:
化学工程
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环境科学
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物理化学
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分离科学
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绿色化工
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yingjie Niu,Shiying Zou,Haonan Liu,Minyue Hu,Jinjun Cai,Chao'en Li,Kathryn A. Mumford,Masood S. Alivand,Francesco Barzagli,Rui Zhang
Improving the energy efficiency of CO 2 desorption remains a key challenge in post-combustion carbon capture using amine solvents. In this work, a series of solid acid catalysts based on sulfonated mesoporous SBA-15 and functionalized with phosphotungstic acid (HPW) were synthesized via post-synthetic modification and applied to the catalytic regeneration of monoethanolamine (MEA). The catalysts, featuring both Brønsted and Lewis acid sites, were thoroughly characterized and tested in desorption experiments using CO 2 -loaded MEA solutions. Among the synthesized materials, HPW-SBA-15-SO 3 H-1 exhibited the best performance, achieving significantly higher CO 2 desorption rate and cyclic capacity compared to the uncatalyzed system, while reducing the relative heat duty by up to 37.7 %. This catalyst also demonstrated good stability over 20 absorption–desorption cycles, maintaining its structural integrity. In addition, machine learning was employed to correlate the catalysts' physicochemical features with their desorption performance, highlighting the role of acidity and porosity and supporting the proposed mechanism by which acidic sites promote carbamate decomposition and MEAH + deprotonation. These findings underscore the potential of functionalized mesoporous silica as efficient solid catalysts for lowering the regeneration energy penalty in MEA-based carbon capture systems.
研究领域:
化学工程
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材料科学
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环境科学
·
催化
·
机器学习
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Ye Yuan,Jia Hu,Yu Wang,Leilei Huang,Jiayun Zheng,Yufeng Zhao,Yiyun Chen,Cheng Chen,Francis Verpoort
α-Hydroxy ketones are important building blocks in biological, pharmaceutical and synthetic chemistry. In this work, diverse α-hydroxy ketones were efficiently constructed through the CO 2 -promoted hydration process of propargyl alcohols, which was catalyzed by a system consisted of economical CuSO 4 ·5H 2 O and a green 1-butyl-3-methylimidazolium acetate ionic liquid. Particularly, this catalytic system exhibited excellent activity under atmospheric CO 2 or even mimetic flue gas (20 vol% of CO 2 ). Moreover, this system employed the lowest metal loading ever reported (0.004–0.25 mol%) meanwhile reached the highest turnover number (11700) for the target hydration reaction. Additionally, this is the first reported Cu catalytic system with reliable recyclability, which could be easily reused at least 6 times with yields higher than 85%.
研究领域:
催化
·
绿色化学
·
有机合成
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yan Huang,Yufeng Zhou,Zebin Yu,Shijie Li,Zuofang Yao,Yi Liu,Xinqiu Tan,Yikai Wang,Yanping Hou
To address the bottlenecks of sluggish carrie r separation and insufficient active sites in lead-free halide perovskite of Cs 3 Sb 2 Cl 9 , magnetic transition metal (Co) was introduced and regulated the Co/Sb bimetallic ratio via a facile co-precipitation method to develop the Cs 4 Co 1.2 Sb 1.8 Cl 12 for light-driven CO 2 conversion. Results of electron paramagnetic resonance (EPR), Kelvin probe force microscopy (KPFM) and theoretical calculations revealed that the introduction of Co 2 + could promote the formation of chlorine vacancies ( V Cl ) and enhance local spin polarization, thereby facilitating CO 2 adsorption and activation, as well as accelerating carriers separation. The average carriers lifetime of the Cs 4 Co 1.2 Sb 1.8 Cl 12 was 1.8 times that of pristine Cs 4 CoSb 2 Cl 12 , beneficial to charges participation in CO 2 reduction reaction. The CO yield from the Cs 4 Co 1.2 Sb 1.8 Cl 12 (130.23 μmol·g −1 ·h −1 ) was 1.33 times that of Cs 4 CoSb 2 Cl 12 and 278 times that of pur e Cs 3 Sb 2 Cl 9 . Notably, without sacrificial agent, an unprecedented CO yield of 66.22 μmol·g −1 ·h −1 was achieved in photocatalytic CO 2 reduction, representing the best performance among lead-free halide double perovskites reported to date. In-situ FTIR analysis demonstrated the carboxylate (COOH*) as the dominated intermediate during CO 2 reduction. This work provides a reference for designing efficient lead-free halide perovskite photocatalysts via enriching halide vacancies and strengthening spin polarization for CO 2 conversion.
研究领域:
材料科学
·
光催化
·
钙钛矿化学
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环境科学
·
能量转换
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2015
·
IF 3.562
Xue Jiang,Chun Feng,Guolin Lu,Xiaoyu Huang
A homopolymer strategy was developed to synthesize temperature and pH/CO 2 stimulus-responsive homopolymers. A new class of acrylamide monomers bearing oligo(ethylene glycol) unit and N,N -diethylaminoethyl group were designed and prepared through Aza-Michael addition reaction followed by amidation with acryloyl chloride using amino group as a linkage to connect oligo(ethylene glycol), N,N -diethylaminoethyl, and polymerizable double bond groups together. Subsequently, the corresponding homopolymers containing oligo(ethylene glycol) unit and N,N -diethylaminoethyl group in each repeated unit were prepared via RAFT polymerization with controlled molecular weights and relatively narrow molecular weight distributions . The lower critical solution temperature (LCST) of homopolymer was examined to be influenced by molecular weight, salt concentration, and pH value of aqueous solution. The LCSTs of homopolymers could be tuned in a wide temperature window by changing pH value of aqueous solution and it increased with the decrease of pH value. Particularly, CO 2 gas as a unique pH stimulus can also reversibly adjust the solubility of homopolymer without the addition of acids or bases.
研究领域:
高分子化学
·
智能材料
·
药物递送
·
生物医用材料
·
刺激响应材料
✓ 已验证
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 56
·32358-32367
·
IF 2.936
Yong Dong,Liqin Cao,Jing Li,Yongxia Yang,Jide Wang
A novel clean method to synthesis a composite monolith was developed. Given its amphiphilic property, UiO-66 can emulsify water and CO2 to format a high internal phase emulsion (HIPE) under certain conditions. These UiO-66-emulsified Pickering HIPEs can be used as templates to prepare interconnected macroporous MOF/polymer composite monoliths. The effects of UiO-66 amount, cross-linking agent concentration, and CO2–water ratio on UiO-66/PAM structures were investigated. Then, the as-synthesized MOF/PAM composites were characterized by TGA, XRD, SEM, and FT-IR analyses, as well as rheological and DMA measurements. The results indicated that the composites are interconnected with hierarchical pores, and the diameter of the voids is 10–50 μm. The directly prepared monoliths exhibited relatively high stresses at 82% strain and recovered their shape quickly. The adsorption capacity of the composites for methylene blue (MB) is 50 mg g−1 at a faster adsorption rate. The monoliths also exhibit underlying applications in edible oil–water separation.
研究领域:
材料科学
·
化学工程
·
环境科学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2017
·
IF 3.091
Hongxia Gao,Zeyang Wu,Helei Liu,Xiao Luo,Zhiwu Liang
The absorption/desorption performance of carbon dioxide (CO2) in aqueous 5 M monoethanolamine (MEA) solutions in the presence of various solution regeneration promoters was comprehensively investigated using a multiple rapid screening method. The promoters considered were N-methyldiethanolamine (MDEA), N,N-dimethylethanolamine (DMEA), N,N-diethylethanolamine (DEEA), 1-dimethylamino-2-propanol (1DMA2P), 1-diethylamino-2-propanol (1DEA2P), 3-dimethylamino-1-propanol (3DMA1P), 2-(dimethylamino)-2-methyl-1-propanol (2DMA2M1P), triethanolamine (TEA), 3-(dimethylamino)-1,2-propanediol (3DMA-1,2-PD), and 3-(diethylamino)-1,2-propanediol (3DEA-1,2-PD). The molar concentration of these promoters added into 5 M MEA was set to 1 mol/L. At the atmospheric pressure, the absorption and stripping experiments were carried out at 313.15 and 353.15 K, respectively. Especially, the CO2 partial pressure was controlled at constant 15 kPa for absorption experiments. In addition, the equilibrium solubility of CO2 was also determined in order to evaluate the driving force of each amine system. The results showed that the highest CO2 equilibrium solubility of 0.5548 mol CO2/mol amine was obtained by MEA/1DEA2P, whereas both the fastest absorption and regeneration rates were achieved for aqueous blended MEA/1DMA2P solution which made MEA/1DMA2P to exhibit the highest CO2 cyclic capacity of 1.6710 mol CO2/L.
研究领域:
化学工程
·
环境科学
·
能源技术
·
物理化学
✓ 已验证
DOI
高影响因子
Solids
·
2025
·Vol. 6
·期 3
·49
·
IF 2.4
Xinyue Jing,Minxuan Chen,Xingye Ma,Xinrui Xu,Ning Wang,Kunpeng Niu,Xiaohan Chen,Yihao Wang,Jiayi Zhu,Jianguo Hou,Zhichao Wang
As a vital transition metal species, cobalt ions (Co2+) play a critical role in industrial and medical fields. However, uncontrolled release into ecosystems via industrial effluents presents significant environmental risks. To address this, a prism-coupled surface plasmon resonance (SPR) sensor chip was developed which enables simultaneous high sensitivity, wide detection range, and rapid detection of Co2+under ultra-low detection limit conditions. By depositing a 50 nm Au film and AuNPs on a glass substrate, and integrating carboxyl-functionalized carbon quantum dots (CQDs), the chip achieved the detection range of 10−20mol/L to 10−4mol/L, and the response time was reduced from 21 min to 11 min under optimal electric field conditions (1.2 V, 0.15 mol/L electrolyte concentration). The sensor exhibits high selectivity, repeatability, and stability. It can be integrated with optofluidic technology to enable high-throughput microfluidic analysis, thereby facilitating further advancements in related research.
研究领域:
环境监测
·
传感器与生物传感器
·
纳米材料
·
分析化学
·
光学传感
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）