PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2024
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IF 6.9
You-yun Gong,Zi-ang Jia,Yiwen Fan,Jin-ping Cheng
Rational chemical modification engineering of metal-organic frameworks (MOFs) is an effective means to improve their CO 2 capture efficiency. In this study, we prepare UiO-66 MOF impregnated with different types of aliphatic amines using solvothermal and impregnation techniques, respectively, and investigated their performances in CO 2 adsorption and CO 2 /N 2 separation using the isothermal adsorption method. Aliphatic amines successfully chemically modifies UiO-66, and their molecules effectively occupied the pores of the UiO-66 framework, which has been confirmed by material characterization, experiments, and DFT-FMO calculations. There are significant improvements in the ability to capture CO 2 when aliphatic amines were added to UiO-66 compared to pure UiO-66 (1.39 mmol/g up to 2.11 mmol/g-2.53 mmol/g), attributed to the different types and numbers of amines, and there were also differences in the Zr metal clusters and BDC ligands. Meanwhile, The material has better CO 2 /N 2 adsorption IAST selectivity(98) because its surface area is changed and N 2 does not interact specifically with the adsorbent. Furthermore, the CO 2 adsorption capacity remains constant across multiple adsorption cycles, highlighting the adsorbent's stability and reliability during repetitive CO 2 capture. This study provides new ideas and perspectives for improving the CO 2 capture efficiency of UiO-66.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Zhihe Zhang,Zihang Yu,Kai Feng,Binhang Yan
CO 2 methanation is gaining renewed attention due to the emerging application needs such as the power-to-gas concept and long-term space exploration missions. Maximizing the amounts of interfacial sites generally regarded as the efficient active sites is considered to be one of the most direct means to enhance catalytic activity but few breakthroughs have been made. Here, Eu 3+ is introduced to Ni/CeO 2 to promote the Ni-CeO 2 interaction, resulting in a remarkable low-temperature CO 2 methanation activity. Structural characterization indicates that the Ni/CeEu(9:1) catalyst achieves higher Ni dispersion compared to Ni/CeO 2 , which consequently generates more interfacial sites. More interfacial sites enhance the proportions of bidentate carbonates closer to interfacial sites as a faster hydrogenated species during the catalytic process, leading to enhanced low-temperature CO 2 methanation activity over the Ni/CeEu(9:1) catalyst. This work provides a chemical strategy to enhance the amounts of active sites and bring insights into the origin of enhanced catalytic performance.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2011
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IF 2.089
Jun Li,Yinmei Ye,Lifang Chen,Zhiwen Qi
The solubilities of CO2 in solvent poly(ethylene glycols) (PEGs) with molecular weights of 150, 200, 300, and 400 were measured over the range of pressure from (100 to 1200) kPa and temperature from (303.15 to 333.15) K. Henry's constant was obtained by linear fitting of the experimental data, and thermodynamic properties of solutions were calculated from the correlation of Henry's constant. It indicates that the solubility of CO2 increases with increasing molecular weights of PEGs. Henry's constant based on mole fraction and the molality of CO2 in PEG400 vary from (4.78 to 7.09) MPa and (1.56 to 2.48) MPa·kg·mol–1 from (303.15 to 333.15) K, respectively.
研究领域:
化学工程
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物理化学
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2023
·Vol. 17
·期 1
·297-306
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IF 9.9
Xie Jing,Lu Zhenjiang,Feng Yue,Huang Jianguo,Hu Jindou,Hao Aize,Cao Yali
Defect modulation currently plays a decisive role in addressing the poor photoabsorption, sluggish electron hole separation, and high CO 2 activation barrier in photocatalytic CO 2 reduction. However, hunting for a straightforward strategy to balance the concentration of oxygen vacancy and metal cation defect in one photocatalyst is still a great challenge. Herein, a bismuth vacancies BiOBr nanosheets (BiOBr-1) on the exposed [001] facets were constructed via an acetic acid molecule modification strategy, which can repair oxygen defect by bismuth vacancy in low-temperature solid-state chemical method. Benefiting from the formed bismuth defects that can not only broaden light absorption and elevate charge separation efficiency, but also enhance adsorption and activation of CO 2 molecules, the evolution rates of photocatalytic CO 2 conversion into CO (71.23 µmol·g −1 ·h −1 ) and CH 4 (8.90 µmol·g −1 ·h −1 ) attained by BiOBr-1 are superior 7.1 and 11 times to that of plate-like BiOBr. The photocatalytic mechanisms including adsorption concentration and activation process of CO 2 are further revealed by the in situ diffuse reflectance infrared flourier transform spectra (DRIFTS). This finding of the existence of distinct defects in ultrathin nanosheets undoubtedly leads to new possibilities for photocatalyst design using two-dimensional materials with high solar-driven photocatalytic activity.
研究领域:
材料科学
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环境科学
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纳米技术
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催化
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物理化学
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2025
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IF 14.3
Wenjiao Chang,Honghuo Wang,Tingting Wu,Shuting Zhang,Yifan Li,Junying Wang,Yongqiang Yang,Lei Wang
Photocatalytic CO 2 reduction reaction is regarded as a potential strategy to convert greenhouse gases into valuable chemicals. However, achieving photocatalysts with high efficiency and target product selectivity under visible light still faces great challenges. Herein, sub-2 nm RuO 2 @TiO 2 (RTO) nanorods with lattice matching interface are rationally designed and prepared via a hydrothermal reaction step-by-step. Due to the strong interaction of the lattice-matched interface with the Ru-O-Ti bond, new energy levels have emerged at the interface, leading to effective visible light absorbance. Moreover, the photo-generated electrons could be transferred to the RuO 2 efficiently via the lattice-matched interface. As a result, the RTO photocatalyst exhibits superior CO 2 -to-CH 4 conversion performance of 15.6 µmol g −1 with a selectivity of 87.9% under visible light irradiation. Density functional theory (DFT) calculation reveals that the energy barrier of CO* to CO is significantly higher than that of *CHO, resulting in the preferential production of CH 4 . This work provides an effective strategy for designing photocatalyst with promoted visible light absorption and improved product selectivity.
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ChemPhotoChem
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2025
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IF 3
Mengrong Zhang,Sha Ni,Zichao Yang,Min Zhang,Zhongjie Guan,Jianjun Yang
Graphical Cu-modified monoclinic TiO 2 nanoflowers with OVs (Cu 1 TB-1.5) promote the reactivity and selectivity of CO 2 reduction to CO under visible light. CO selectivity is 99.6%, and the cycling stability is excellent. The Cu 1 TB-1.5 facilitates the formation of the intermediate COOH* during the photocatalytic process, thus improving the yield and selectivity of CO. The photoreduction of CO 2 has attracted extensive attention as a promising solution to global warming. In this study, Cu-modified TiO 2 (B) (CuTB) nanoflowers with oxygen vacancies (OVs) are designed and synthesized via hydrothermal treatment and photodeposition to promote the reactivity and selectivity of CO 2 reduction to CO under visible light. The CO and CH 4 yields of sample Cu 1 TB-1.5 under visible light are 5.72 and 0.02 μmol g −1 h −1 , wherein the CO yield was 15.5 times that of sample TB; its selectivity is 99.6%, and the cycling stability is excellent. OVs can broaden the light absorption of TB to the visible light region, and Cu promotes photoinduced electron transfer from TB to the Cu species and act as an active center. The OVs and Cu can synergistically enhance charge separation, CO 2 adsorption, and CO 2 conversion. The Cu 1 TB-1.5 facilitates the formation of the intermediate COOH* during the photocatalytic process, thus improving the yield and selectivity of CO. This research provides a unique idea for the development of novel highly selective photocatalysts.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Fanwei Meng,Chao Qu,Lanyang Wang,Decai Yang,Zezhong Zhao,Qing Ye
Photocatalytic CO 2 reduction technology plays a significant role in the energy and environmental sectors, highlighting the necessity for developing high-efficiency and stable catalysts. In this study, a novel photocatalyst, x NiCo 2 O 4 /CN ( x = 1, 3, and 5 wt%), was synthesized by depositing zeolitic imidazolate framework-67 (ZIF-67)-derived nickel cobaltate (NiCo 2 O 4 ) hollow nanocages onto porous graphitic carbon nitride ( g -C 3 N 4 , CN) nanosheets for photocatalytic CO 2 reduction. Under visible light irradiation, the resulting 3NiCo 2 O 4 /CN photocatalyst demonstrated exceptional CO yields of up to 2879.5 μmol g −1 h −1 , surpassing those of NiCo 2 O 4 and CN alone by factors of 3.3 and 11.6, respectively. The introduction of hollow NiCo 2 O 4 nanocages increased the specific surface area of the material and enhanced the number of active sites, while strengthening visible light absorption. The creation of a built-in electric field, induced by the Fermi level difference between the two materials, was confirmed through ultraviolet photoelectron spectroscopy (UPS) characterization. This resulted in the formation of a Z-scheme heterojunction, significantly enhancing the separation and migration of photogenerated charge carriers. Notably, 3NiCo 2 O 4 /CN exhibits excellent stability during long-term photocatalytic reactions, ensuring reliable performance for practical applications. This study offers novel insights and methodologies for developing efficient photocatalytic CO 2 reduction catalysts.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2024
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IF 6.7
Wenxia Wang,Yuliang Zhu,Yingchao Hu
High-temperature CO 2 capture based on Li 4 SiO 4 sorbents has been well recognized as an effective approach to mitigate the global warming issues. However, the relatively low sorption performance is one of the biggest challenges for the practical application. In the current investigation, Na- and Y-based dopants have been employed to enhance cyclic CO 2 sorption performance of Li 4 SiO 4 sorbents. Various physicochemical properties and cyclic CO 2 sorption performance of the prepared sorbents have been systematically studied. The results indicated that Na 2 CO 3 and Y 2 O 3 codoped Li 4 SiO 4 sorbent (Li 4 SiO 4 -10Na-15Y) exhibited excellent cyclic CO 2 capture performance with stable capacity of >0.27 g CO 2 /g sorbent (corresponding to the carbonation conversion of ∼96 %) during 15 sorption/desorption cycles. Even under lower CO 2 concentration and longer cycles, satisfying conversions of 85 % could be kept in the cyclic tests for the codoped Li 4 SiO 4 sorbent. In addition, the materials also showed high heat storage density of 557.8 kJ/kg and the performance was stabilized in the multicycle energy storage/release tests. The characterization results showed that the introduction of Y-based dopants induced triple positive effects for Li 4 SiO 4 including porosity creation, sintering-resistant ability, and producing Li 4 SiO 4 lattice defects. As a result, the enhanced specific surface area and reduced diffusion resistance were achieved and, thus, the CO 2 sorption performance including sorption capacity (heat storage density) and cyclic stability was obviously improved.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Maijun Li,Yubo Long,Zhibo Zheng,Xu Hu,Siwei Liu,Zhenguo Chi,Nanwen Li,Jiarui Xu,Yi Zhang
Chemical modification of polyimide membranes is employed to achieve “trade-off” breakthrough or improve the plasticization resistance in CO2 separation. However, harsh reaction conditions restrict the application of traditional chemical modifications. In this work, a simple chemical modification method─the coordination cross-linking between hydroxyl groups on polyimide (6FSPI) and Zn(II)─was investigated. Because of the reversible complexation of Zn(II) in the modified membrane as a transport carrier with CO2, and the addition of Zn(II) disrupts coiled chain of spiro moiety or intrachain cross-linking to induce more quantities of ultrafine micropores, the CO2 permeability coefficient of the modified membrane is 2.97 times that of the pristine 6FSPI. Simultaneously, there is improvement in diffusion selectivity of the modified membrane, resulting in the CO2/CH4 selectivity improvement. The overall CO2/CH4 separation performance of the modified membrane reaches up to the 2008 Robeson limit. In addition to serving as facilitated transport carriers, Zn(II) can also be used as cross-linking points. The modified membrane maintains a stable CO2 permeability coefficient beyond 4000 kPa. Our work suggests that the Zn(II) coordination cross-linking is a facile chemical modification method that can enhance long-term performance and separation performance of polyimide membranes simultaneously.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2018
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IF 3.849
Yafei Guo,Chang Tan,Peng Wang,Jian Sun,Junjie Yan,Weiling Li,Chuanwen Zhao,Ping Lu
Coal and biomass fly ash was impregnated with tetraethylenepentamine (TEPA) to prepare solid CO 2 sorbent. Experimental CO 2 adsorption capacities of the sorbent in fixed-bed column were fitted to several kinetic equations. The modified Avrami fractional kinetic model could accurately predict the CO 2 adsorption kinetic behaviors of the sorbent under different conditions. CO 2 adsorption rate increases with the increase in temperature, initial CO 2 concentration and gas flow rate, as a result of the decreased CO 2 diffusion resistance. A mathematical model was proposed and demonstrated to well predict the CO 2 adsorption breakthrough curves in the fixed-bed column. Effects of temperature, initial CO 2 concentration and gas flow rate on the mass transfer kinetic behaviors of the desired sorbent were investigated. The positive effect of these factors on promoting the overall mass transfer coefficient and the internal mass transfer coefficient is not significant. The external mass transfer coefficient will be remarkably reinforced with the increase in these operating parameters, due to the change in viscosity and density of the gas phase and the reduced external mass transfer resistance. Internal mass transfer process is determined as the rate-limiting step for CO 2 adsorption. The results will lay the groundwork for future scale-up application of the sorbent in post-combustion CO 2 capture.
研究领域:
环境科学
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化学工程
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能源工程
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大气污染控制
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碳捕集与封存
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shuangxi Lin,Longchen Gong,Ning Zhao,Huibo Zhao,Feigang Zhao,Yang Bai,Zhenhua Li,Wen Liu
Modulating metal-support interactions is critical for improving catalytic activity and product selectivity for CO 2 hydrogenation. Such modulation can be achieved by modifying the metal nanoparticles as well as the supports. Here, we prepared a novel catalyst, in which Ni nanoparticles were dispersed on CeO 2 and hexagonal boron nitride (h-BN) hybrid supports. The introduction of h-BN to Ni/CeO 2 -BN effectively improves the dispersion of Ni nanoparticles. More importantly, the abundant Ni-CeO 2 interfacial sites with enriched oxygen vacancies are formed over h-BN edge sites. The dispersed Ni species are anchored on CeO 2 via a unique interfacial structure, with electron-rich Ni (Ni δ− ) species. At the interfacial sites on Ni/CeO 2 -BN, the synergy between oxygen vacancies and Ni δ− , which enhances CO 2 activation and H 2 dissociation, respectively, renders superior catalytic performance for CO 2 methanation. In situ DRIFTS suggests formate as key rate-limiting intermediates on Ni-CeO 2 sites, while the formation of B-H bonds further promotes hydrogen activation and subsequently the catalytic performance. The modulation of metal-support interactions by spatial confinement effect by BN offers a new paradigm for designing metal/oxide catalysts for chemical transformations that requires bifunctionality as CO 2 hydrogenation.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2024
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IF 4
Longting Qi,Yujing Xie,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Bi 2 MoO 6 has drawn considerable attention in the field of photocatalysis owing to its excellent visible light response and photo-generated carriers transport ability. However, pure Bi 2 MoO 6 suffers from the limited surface-active sites and poor photogenerated charge separation efficiency, resulting in unsatisfactory photocatalytic performance. Herein, the 2D/2D Bi 2 MoO 6 /BiOBr Z-scheme heterojunction photocatalysts were synthesized by in-situ hydrothermal growth of Bi 2 MoO 6 on BiOBr. The optimized heterojunction catalyst, Bi 2 MoO 6 /BiOBr-40 % exhibited a CH 3 OH yield of 6.21 μmol·g -1 ·h -1 , which was twice that of the pure Bi 2 MoO 6 . Simultaneously, mechanism study by the band potential estimation and electron spin resonance (ESR) analysis evidenced that the enhanced activity was ascribed to the Z-scheme. This unique structure could enhance the spatial separation of electron-hole pairs, remain the strong redox ability. Moreover, the density functional theory (DFT) calculations were carried out to further expose the charge transfer mechanism of composites. This paper provided a novel approach for the design and manufacture of 2D/2D Z-scheme heterojunctions for energy conversion and environmental remediation.
研究领域:
材料科学
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环境科学
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能源科学
✓ 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）