JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Jing Lei,Wei Bi,Mitang Wang,Hao Jiang,Yanjie Hu,Chunzhong Li
How to achieve controllable preparation of heterostructure and in-situ optimize the interface and internal electron transfer by a fast and economic synthesis method has become a big challenge in the practical application of photocatalysis. Herein, an island-shaped SrTiO 3 (STO) perovskite nanodots and TiO 2 (T) compounded S-scheme SrTiO 3 /TiO 2 (ST) heterostructure was successfully developed. During the millisecond reaction process, the decomposed Sr 2+ penetrated into the TiO 2 lattice causing the lattice expansion and inducing local atomic rearrangements, resulting in the generation of STO phase. Owing to the synergy of the efficient electron transport at the perovskite nanodots interface and the stronger reduction capacity, the performance of the optimized ST1 sample is greatly improved to 86.90 μmol g −1 for CO 2 -to-CO and 21.31 μmol g −1 for CO 2 -to-CH 4 . The utilization of electrons reached up to 119.74 μmol g −1 h −1 , which was 3.13 times higher than that of T. Detailed characterizations and density functional theory (DFT) calculations proof that the formation of intermediates HCOO − and CO 3 2− is the key to the performance improvement critically. Overall, this work originally reports a feasible strategy for flame synthesis of S-scheme heterostructure photocatalyst.
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WATER RESEARCH
·
2025
·
IF 12.4
Lei Zhou,Dian Wang,Jiayu Yu,Hongyi Zhang,Hang Dong
Nitrogen recovery from urine and CO 2 utilization are both vital for achieving a circular economy and mitigating climate change. Divided engineering solutions have been proposed to address either problem, but there is still a lack of integrated technologies to simultaneously tackle the two tasks. We demonstrated CO 2 -driven ion exchange for nitrogen recovery (CIXNR) from urine and evaluated the process in Malawi. By comprehensively studying the ion exchange chemistry using a proton-form weak acid cation exchanger (WAC-H), we revealed the suppressed adsorption capacity caused by counterion releasing. Regulating aqueous pH optimized the WAC-H capacity, particularly, by the natural buffering capacity provided by bicarbonate in the hydrolyzed urine. CO 2 regeneration achieved over 75 % nitrogen recovery in a multi-cycle test with synthetic hydrolyzed urine. A higher CO 2 pressure resulted in faster regeneration kinetics due to a lower aqueous pH and higher proton concentration gradient. Our field outreach activity in Malawi indicated future research demand in adapting the system for resource-limited, rural, and no-electricity areas. We envision this study to inspire more integrated solutions to tackle both circular economy and climate actions and call for more field outreach activities to facilitate urine technology adoption in developing countries.
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VACUUM
·
2025
·
IF 3.9
Jingwen Meng,Xiaoli Jin,Mengyuan Zhao,Zhuohua Chen,Weixi Hao,Shilong Lin,Xin Li,Fengyun Su,Fei Li,Kaiting Yang,Xiongtao Lv,Xuhan Zhang,Haiquan Xie
Limited light absorption and low carrier separation efficiency remain major obstacles to converting CO 2 into solar fuel. Rational design of semiconductor photocatalysts with unique structures holds promise for overcoming these challenges. In this study, Bi 4 O 5 Br 2 photocatalyst with a hollow core-shell architecture is synthesized via a one-step solvothermal method. This innovative structure facilitates efficient reflection and absorption of incident light within its internal cavity, while also minimizing the charge transfer path. Consequently, it significantly improves both light harvesting capabilities and charge carrier separation efficiency. Compared to the solid Bi 4 O 5 Br 2 (CO, 0.21 μmol g −1 h −1 ; CH 4 , 0.78 μmol g −1 h −1 ) and hollow Bi 4 O 5 Br 2 (CO, 0.25 μmol g −1 h −1 ; CH 4 , 0.99 μmol g −1 h −1 ) counterparts, the hollow core-shell Bi 4 O 5 Br 2 exhibits superior CO 2 photoreduction performance, achieving production rates of 3.61 and 2.40 μmol g −1 h −1 for CO and CH 4 , respectively. Notably, it also enhances C 2 H 4 production during the CO 2 reduction process, with a yield of 0.17 μmol g −1 h −1 , whereas no detectable C 2 H 4 is produced by either the solid or hollow Bi 4 O 5 Br 2 structures. This research provides fresh insights into the structural design of advanced photocatalysts and holds significant implications for converting CO 2 into high-value chemicals.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Xi Chen,Wei Zhou,Xu Fang,Cheng Li,Die Cong,Tie Yu,Wei-Qiao Deng,Chengcheng Liu
Photocatalytic CO2 reduction to syngas has recently garnered substantial interest due to its mild reaction conditions, high safety, and environmental sustainability. However, the efficiency of syngas production remains relatively low. In this study, we have developed metallosalen-based poly(ionic liquid)s (PILs) to enhance syngas production, achieving one of the highest production rates recorded to date. The Co(Salen)-PIL demonstrates a syngas production rate of 168.1 mmol g−1 h−1, including a CO production rate of 69.3 mmol g−1 h−1, which is more than eight times higher than that of the best previously reported organic materials. Mechanistic investigations reveal that pyridine ions facilitate electron transfer from the heptazine light-harvester to the Co(Salen) active site. This study lays the groundwork for developing high-performance catalysts for photocatalytic syngas production.
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CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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2024
·
IF 5.9
Yongheng Ren,Yang Chen,Hongwei Chen,Lu Zhang,Jiangfeng Yang,Qi Shi,Lin-Bing Sun,Jinping Li,Libo Li
The identical molecular size and similar physical properties of carbon dioxide (CO 2 ) and acetylene (C 2 H 2 ) make their adsorptive separation extremely challenging to achieve with most adsorbents. Reports on the separation of CO 2 and C 2 H 2 mixtures by zeolites are even rarer with the mechanism of adsorptive separation requiring further exploration. In this paper, we report that ion modulation of zeolite 5A promotes the difference in kinetic diffusion of CO 2 and C 2 H 2 , realizing the inverse separation of zeolite from selective adsorption of C 2 H 2 to selective adsorption of CO 2 . Creating a compact pore space restricting the orientation of gas molecules enables charge recognition. The positive electrostatic potential at the pore openings was utilized to hinder the diffusion of C 2 H 2 between the cages while ensuring the transfer of CO 2 , increasing their diffusion differences in pore channels and leading to the CO 2 /C 2 H 2 kinetic selectivity of 31.97. Grand canonical Monte Carlo (GCMC) simulation demonstrates that the CO 2 distribution in K-5A- β is significantly higher than that of C 2 H 2 . Dynamic breakthrough experiments verify the excellent performance of material in practical CO 2 /C 2 H 2 separation, for CO 2 /C 2 H 2 (50/50 and 1/99, V/V) mixtures can be separated in one step, thus directly generating high purity C 2 H 2 (> 99.95%), which provides a promising thought for the zeolite-based separation of CO 2 and C 2 H 2 .
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MOLECULES
·
2024
·Vol. 29
·期 3
·578
·
IF 4.2
Hengxin Jian,Mengyu Lu,Haowen Zheng,Shengrui Yan,Mei Wang
Mimicking the photosynthesis of green plants to combine water oxidation with CO2reduction is of great significance for solving energy and environmental crises. In this context, a trinuclear nickel complex, [NiII3(paoH)6(PhPO3)2]·2ClO4(1), with a novel structure has been constructed with PhPO32−(phenylphosphonate) and paoH (2-pyridine formaldehyde oxime) ligands and possesses a reflection symmetry with a mirror plane revealed by single-crystal X-ray diffraction. Bulk electrocatalysis demonstrates that complex1can homogeneously catalyze water oxidation and CO2reduction simultaneously. It can catalyze water oxidation at a near-neutral condition of pH = 7.45 with a high TOF of 12.2 s−1, and the Faraday efficiency is as high as 95%. Meanwhile, it also exhibits high electrocatalytic activity for CO2reduction towards CO with a TOF of 7.84 s−1in DMF solution. The excellent electrocatalytic performance of the water oxidation and CO2reduction of complex1could be attributed to the two uniqueµ3-PhPO32−bridges as the crucial factor for stabilizing the trinuclear molecule as well as the proton transformation during the catalytic process, while the oxime groups modulate the electronic structure of the metal centers via π back-bonding. Therefore, apart from the cooperation effect of the three Ni centers for catalysis, simultaneously, the two kinds of ligands in complex1can also synergistically coordinate the central metal, thereby significantly promoting its catalytic performance. Complex1represents the first nickel molecular electrocatalyst for both water oxidation and CO2reduction. The findings in this work open an avenue for designing efficient molecular electrocatalysts with peculiar ligands.Keywords:transition metal complex;water oxidation;carbon dioxide reduction;electrocatalysis;synergistic catalysis
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CATALYSIS LETTERS
·
2024
·
IF 2.3
Liu Hang,Liu Sixu,Liang Yaozhen,Sun Yifei,Xiong Haifeng
Palladium (Pd)-based catalysts are widely used for CO 2 hydrogenation reactions due to the capability to activate H 2 , which enhances the overall CO 2 conversion. However, most of the current Pd catalysts reported show high CO 2 conversion only at higher temperature, and the exploration of efficient catalyst enabling low temperature conversion (180–300 °C) is of importance. In this study, a series of Pd-B/ZnAl 2 O 4 catalysts were synthesized via in-situ doping, resulting in the Pd crystal transformation induced from crystal to amorphous. The catalytic hydrogenation activity of the amorphous Pd-B catalyst reaches its zenith at a Pd-B mole ratio of 1:2, accompanied by the superior catalysis stability in CO 2 hydrogenation. Various characterization techniques, including XRD, CO-DRIFTS, H 2 -TPR, XPS and TEM, were used to investigate the properties of the Pd-B/ZnAl 2 O 4 catalyst. The results showed that the Pd-B/ZnAl 2 O 4 catalyst exhibited higher dispersion and better CO 2 conversion efficiency compared to unmodified Pd catalyst. Additionally, the methanol space–time yields are nearly doubled when the B decoration is employed. At 280 °C, CO 2 conversion was improved and methanol selectivity remained at ~ 65%. This study provides valuable insights into the design and optimization of Pd-B based catalysts for CO 2 hydrogenation at low temperatures. Graphical Abstract
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Jiangnan Wang,Long Li,Jinli Zhang,Xueqin Li
The chitosan (CS)-grafted UiO-66-NH 2 (U6N) (CSGUN) was synthesized and incorporated into Pebax matrix to fabricate mixed matrix membranes (MMMs) for boosting CO 2 transport. The excellent CO 2 separation performance was exhibited for MMMs due to the following reasons: U6N with the suitable porosity and abundant CO 2 transport carriers can provide a unique “expressway” for CO 2 to boost CO 2 transport through MMMs. The grafting CS in CSGUN can connect Pebax (regular roads) and U6N (expressway), acting as an “on-ramp” between them to enrich CO 2 and guide CO 2 through U6N in an orderly manner. Thus, the constructed “on-ramp” and “expressway” in MMMs can improve CO 2 separation performance. Furthermore, the CS-MOF networks were formed in MMMs through using CS molecular chains to connect U6N for enhancing CO 2 separation performance of MMMs. Therefore, Pebax/CSGUN MMMs exhibited the excellent CO 2 separation performance with the CO 2 permeability of 558 ± 7 Barrer and the CO 2 /CH 4 selectivity of 37.5 ± 0.7. The study indicated that MMMs with CS-MOF bridged networks had great potential for boosting CO 2 transport by combining “expressways” and “on-ramp”.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Mingmin Jia,Xiong-Fei Zhang,Yicheng Zhou,Hengyang Mao,Yijiang Zhao,Jianfeng Yao
In this work, Amine-functionalized CNF/UiO-66 (CNF–NH 2 /UiO-66) composite membranes were fabricated by incorporating UiO-66 nanoparticles in the CNF–NH 2 matrix. The CO 2 -facilitated transfer channels can be constructed in the CNF–NH 2 /UiO-66 composite membrane. As a natural polymer material, CNF–NH 2 would absorb water and form a gel-like structure under humidification. The adsorbed water can convert CO 2 into bicarbonate ions (HCO 3 − ) through the catalysis of amino groups on CNF–NH 2 . Moreover, in CNF–NH 2 /UiO-66 composite membranes, HCO 3 − could quickly migrate to the permeate side promoted by the porous UiO-66, facilitating CO 2 transport. The optimum membrane gave a CO 2 permeability of 257.0 Barrer with a CO 2 /CH 4 ideal selectivity of 71.3.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2012
·Vol. 26
·期 11
·600-603
·
IF 2.061
Dongsheng Bai,Huanwang Jing,Guangjian Wang
The synthesis of cyclic carbonates from epoxides and carbon dioxide catalyzed by cyanocobalamin and n -Bu 4 NI system was achieved under 0.8 MPa CO 2 pressure at 140°C without organic solvents. Propylene carbonate was obtained in 99% yield within 6 h under the optimized reaction conditions. The cyanocobalamin catalyst could be recycled with water and retained moderate catalytic activity. Copyright © 2012 John Wiley & Sons, Ltd.
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Small
·
2024
·Vol. 20
·期 34
·2401914
·
IF 13
Zhaohui Fang,Xiaoyang Yue,Quanjun Xiang
Metal halide perovskite quantum dots (QDs) are widely studied in the field of photocatalytic CO 2 due to their strong light absorption and long carrier migration length. However, it can not exhibit high catalytic performance because of the radiative recombination and the lack of effective catalytic sites. Metal organic frameworks (MOFs) encapsulated QDs can not only solve the aforementioned problems, but also maintain their own unique characteristics with ultra-high specific surfaces area and abundant metal sites. In this work, lead-free bismuth-based halide perovskite QDs are encapsulated into Zr-based MOF (UiO-66), which combines the advantages with high power conversion efficiency of QDs and the high surface area and porosity of UiO-66. In addition, benefiting from the close contact between the Cs 3 Bi 2 Br 9 QDs and the UiO-66 enables the photogenerated electrons in the QDs to be rapidly transferred to the MOF. As a result, the Cs 3 Bi 2 Br 9 @UiO-66 composite exhibits a higher yield for photocatalytic CO 2 reduction than that of the prepared large-sized composite of Cs 3 Bi 2 Br 9 and UiO-66.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Weida Chen,Meisi Chen,Bin Jiang,Tong Lei,Feng Zhang,Zhibing Zhang
Biphasic absorbents composed of tetraethylenepentamine, 1-ethylimidazole, and H 2 O (TEH) exhibit notable absorption rates and CO 2 loads. However, troublesome precipitation forms in the enriched phase due to strong interactions among absorption products. To address this issue, six amino acid ionic liquids (AAILs) were introduced as split-phase regulators in TEH, developing a liquid–liquid biphasic absorption system TEH-AAILs, with outstanding absorption performance. By analyzing the kinetic data and establishing the evaluation parameters, combined with molecular dynamics simulations, the effects of AAILs on the loading and phasing performance were assessed. Remarkably, TEH-[Ser] was screened to possess good performance. Spectral analysis of the TEH-[Ser] reaction mechanism further elucidates the bridged hydrogen bonding structure between [Ser]–CO 2 and H 2 O, highlighting its role in enhancing regeneration efficiency. This study provides insights into the design and optimization of biphasic absorbents for efficient CO 2 capture.
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