RSC Advances
·
2025
·Vol. 15
·期 11
·8541-8552
·
IF 4.6
Hui Zhang,Yi Hui Sun,Sheng Li An,Rui Hua Guo,Rui Fen Wang,Yu Wei Ma
S-type heterojunction photocatalysts (CeCux-BTC/CN) of cerium-copper bimetallic organic framework (CeCux-BTC) and graphitic carbon nitride (g-C3N4) were constructed by a simple solvothermal method using cerium nitrate, copper nitrate, and urea as the raw materials, and 1,3,5-benzene-tricarboxylic acid as the ligand for the photocatalytic CO2 reduction to CO and CH4. The results show that the built-in electric field constructed by Fermi energy level flattening transfers the electrons in an S-type manner, which not only preserves the strong reducing properties of the electrons in the material but also provides the maximum redox capacity and enables the composite samples to obtain higher visible-light trapping capacity and improve the separation efficiency of the carriers while refining the crystal particles. With the addition of only 1 mL of H2O as the proton supply source, CeCu0.05-BTC/CN exhibits the optimal photocatalytic performance. The CO and CH4 yields were 64.44 and 0.5575 μmol g−1, which were 7.56 and 2.42 times higher than those of g-C3N4, respectively, and the catalytic performances were basically stable after cycling tests.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Lei Wang,Chenhui Qiu,Ruijie Chen,Xueru Chen,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic conversion of CO 2 to renewable clean fuels was a promising way to alleviate the energy crisis and solve environmental issues. However, it remained significantly challenging for designing highly efficient photocatalysts. Herein, the solid solution BiOBr 1-x Cl x (0 ≤ x ≤ 1, BOBC-n, n represented the amount of molten salt) with (001)/(102) facet junction was constructed through a molten salt method. In situ photochemical probing demonstrated that distinct exposed facets allowed photogenerated holes and electrons to migrate to the dominantly exposed and co-exposed facets and thus exhibited different reactivity. Benefiting from facet junction, the optimized BOBC-0.5 exhibited the superior performance of photocatalytic CO 2 to CH 3 OH (5.52 μmol·g −1 ·h −1 ) to that of BiOBr with (001)/(110) facet junction (1.78 μmol·g −1 ·h −1 ). The density functional theory (DFT) calculations further confirmed the separation path of photogenerated carriers between distinct facets, which realized the effective spatial separation of electrons and holes. Moreover, the (102) facet revealed superior adsorption energy of CO 2 molecules to that of (110) facet. This work highlighted a molten-salt strategy to build facet junction for boosting photocatalytic CO 2 performance.
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Journal of Energy Chemistry
·
2024
·
IF 14
Yuan Zhuang,Kaixuan Wei,Zhenxing Li,Hanzhang Gong,Jianan Deng,Haozhong Yuan,Haoyu Lian,Hao Zheng,Honghao Zhao,Xiao Zhang,Jian Liu
Designing the coordination environment of heteroatoms around metal sites and optimizing the electronic structure of diatomic metal sites remain significant challenges in achieving efficient CO 2 overall splitting. Herein, we report four configurations (Cu/Ni–N 4 C 2 , Cu/Ni–N 2 C 4 , Cu/Ni–N 2 C 3 and Cu/Ni–N 2 C 2 ) constructed by precise regulation of the coordination environment around bimetallic atoms. Cu/Ni–N 2 C 2 showed high performance in electrochemical CO 2 reduction (ECR) and water oxidation evolution reaction (OER). In the electrochemical CO 2 overall splitting reaction, it achieved a Faraday efficiency of CO (FE CO ) of 98.0% at a low cell voltage of −2.9 V, significantly higher than widely reported values. Moreover, the FE CO is above 90% over −2.7 to −4.1 V of cell voltages. Cu/Ni–N 2 C 2 achieved long-term ECR stability of 110 h at −100 mA cm −2 . Mechanism studies revealed that the change of coordination environment around the diatomic pairs moves the d-band center of the Ni atom closer to the Fermi level, thereby modulating the adsorption capacity of the catalysts to the reaction intermediates *COOH and *O. This work presents valuable insights into the rational design of diatomic catalysts and elucidates the intricate structure-performance relationship in advancing electrochemical CO 2 overall splitting technology and energy-conversion applications.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Fei Shi,Qinghua Li,Ye Yuan,Yi Yang,Xingzhong Cao,Menglong Sheng,Song Zhao,Zhi Wang
Interfacial polymerization (IP) has been received as an indispensable technology to fabricate thin-film composite (TFC) membranes for gas separation because of the simple and designable process. However, achieving the highly permeable polyamide (PA) TFC membrane for CO 2 capture via the IP technique remains challenging. Herein, a highly CO 2 -permeable PA TFC membrane was synthesized by the polycondensation of N, N-Bis [3-(methylamino) propyl]methylamine (BMAPAm) and trimesoyl chloride (TMC). The ultrathin (∼47 nm) PA TFC membrane featuring with high free volume exhibited excellent CO 2 permeance with moderate CO 2 /N 2 selectivity. The causes of this desired structure were systematically investigated from the aspects of monomer supply and molecular structure, in which the 3,3′-diamino-N-methyldipropylamine (DNMDAm) was used as a comparison. The results illustrated the underlying monomer-structure-performance relationships of IP-made membranes, demonstrating the solid potential of the IP technology specifically toward high-performance CO 2 capture membranes. Finally, a pilot-scale continuous membrane fabrication process was demonstrated.
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Molecular Catalysis
·
2024
·
IF 3.9
Tao Liu,Youcai Zhu,Yue Mu,Xindi Feng,Zhen Liu
CO 2 -based polyols have a unique terminal hydroxyl group structure that makes them suitable for the production of high-performance polyurethane foams. Zn-Co double metal cyanides (DMC) are an important class of catalysts for the copolymerization reaction of CO 2 with propylene oxide (PO). In the DMC-catalyzed CO 2 /PO copolymerization to produce CO 2 -based polyols, the crucial role of chain transfer agents (CTAs) is emphasized. In this work, a high-performance composite CTA (c-CTA) was successfully developed by investigating various dicarboxylic acids and polypropylene glycol (PPG-400) as CTAs. This system combines the high reaction rate of the DMC/PPG-400 system with the high CO 2 insertion rate of the DMC/sebacic acid (SA) system, achieving 2-3 times higher activity than that of single CTA (PPG-400 or SA), reaching 0.5 kg/g. The molecular characteristics of the CO 2 -based polyols synthesized by different DMC/CTAs systems were analyzed by FTIR and 1 H NMR. The reasons for the high catalytic activity of the DMC/c-CTA system were elucidated by analyzing the hydrogen bond distribution in each DMC/CTA systems. Overall, this work provides a theoretical guidance for the development of novel CO 2 -based materials with high industrial application value.
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Nature Communications
·
2026
·
IF 18.1
Jiang Minwen,Liu Chang,Du Zhongyang,Tan Weiwei,Zheng Sihan,Liu Hai,Liu Pingying,Jiang Hejin,Lin Zhixing,Yao Changhong,Wang Fengzhong,Sun Peipei,Zhou Jiajing
The accelerating global energy demand, coupled with diminishing fossil fuel reserves and growing carbon emissions, underscores the urgent need for sustainable energy solutions. Autotrophic microalgae are promising cell factories for converting CO 2 into renewable biofuels. However, conventional microalgal biofuels typically depend on energy-intensive or nutrient-deficient regimes that suppress microalgal proliferation, resulting in a critical trade-off between biomass growth and lipid biosynthesis. Here, we report a separable living interface with microalgae (SLIM) platform that employs extracellular-matrix-mimicking hydrogel scaffolds to spatially organize microalgae and dynamically reconfigure their microenvironment, enabling spatiotemporal switching between biomass accumulation or lipid induction. The SLIM platform supports high-density growth of microalgae while facilitating precision substrate-driven metabolic regulation, enabling low-carbon operation and improved lipid production (8.89 g L −1 ). This work establishes an engineered living material that overcomes essential bottlenecks in microalgal biofuel production and offers a generalizable blueprint for biohybrid systems in advanced biomanufacturing.
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Green Energy & Environment
·
2024
·
IF 10.7
Junming Zeng,Yongbin Yao,Fang Wang,Jiajian Gao,Lili Zhang,Guangwen Xu,Ziyi Zhong,Fabing Su
Nickle-based catalysts are commonly used for CO 2 methanation. However, there is still potential to improve their catalytic performance under mild conditions. In this study, we synthesized a series of Ru-Ni-Al catalysts from Ru-doped NiAl-hydrotalcite using a hydrothermal method. The Ru-Ni-Al catalyst demonstrated much higher activity for CO 2 methanation than the Ni-Al catalyst that did not have Ru doping. Both experimental results and theoretical calculations indicate that the enhanced performance of the Ru-Ni-Al catalyst is related to electronic interactions between nickel (Ni) and ruthenium (Ru). The Ru sites transfer electrons to the Ni sites, increasing the local electron density of Ni, which enhances the adsorption and activation of H 2 . Furthermore, the Ru-Ni metal interface sites improve the adsorption and activation of CO 2 . In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis indicates that adjusting the electronic structure of Ni sites can accelerate the production of intermediates HCOO*, while Ru-Ni intermetallic interface sites can directly dissociate CO 2 into CO*. In addition, CO 2 methanation on the Ru-Ni-Al catalyst follows HCOO*- and CO*-mediated pathways. This study underscores the potential for enhancing CO 2 methanation performance by modulating the electronic structure of Ni sites.
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Energy Technology
·
2024
·Vol. 12
·期 9
·2400114
·
IF 3.6
Jianchao Han,Zihan Qiu,Yuyan Chen,Xia Gui,Xiao Chen
Excessive carbon dioxide (CO 2 ) emissions can lead to environmental problems, and the use of phase change absorbents for CO 2 capture has received much attention due to their excellent absorption and desorption properties. Herein, a novel liquid–liquid phase change absorbent consisting of N-aminoethylpiperazine (AEP), diethylene glycol dimethyl ether (DEGDME), and H 2 O is utilized. Under the optimal absorption conditions, the absorption capacity is 1.23 mol CO 2 ·mol −1 amine. The rich-phase viscosity of the AEP/DEGDME/H 2 O solution is only 6.2 mPa s −1 , and the rich phase-to-volume ratio is 52.7%, which is suitable for industrial applications. After five cycles of absorption–desorption experiments, the cyclic capacity reaches 0.62 mol CO 2 ·mol −1 amine. However, it should be noted that this leads to an increase in the viscosity of the solution with time. The 13 C Nuclear Magnetic Resonance characterization is used to analyze the material distribution and phase separation mechanism, and it is found that during the absorption process, the carbamate and carbonate products generated by the reaction of the amino group in the AEP with CO 2 are mainly located in the rich phase, while the DEGDME and H 2 O mainly remain in the lean phase. In the desorption process, most of the absorbed products are decomposed, and the regeneration efficiency is 66.8%. Through the regeneration energy consumption experiment, when the regeneration efficiency is 56%–67%, the total regeneration energy consumption is 2.71–2.89 GJ t −1 CO 2 , which is 0.91–1.09 GJ t −1 CO 2 lower than that of the regeneration efficiency of 30 wt% MEA solution at 63%, which indicates that this absorbent has certain energy-saving advantages.
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2024
·
IF 2.2
Yong Yang,Peng Yan,Dan Wang,Fang Xie,Dengmeng Song,Ning Wang,Jun Li
Graphical The A 2 B 2 -type Zn-porphyrin containing vinyl and imidazolium groups was utilized for copolymerization with divinylbenzene to prepare metalloporphyrin-based porous organic polymers. Due to the high specific surface area and the coexistence of Zn 2+ and I − , the as-prepared ZnPorI 2 /nDVB exhibited excellent catalytic activity and stability for the cycloaddition of CO 2 and epoxides. In this work, the A 2 B 2 -type Zn-porphyrin (ZnPorI 2 ) featuring vinyl and imidazolium groups was utilized to prepare porous organic polymers (POPs). The vinyl group served as the linking unit for copolymerization with rigid divinylbenzene (DVB). The imidazolium group introduced iodide ions (I − ) into ZnPorI 2 /nDVB (n=30, 50) as Lewis base. By fine-tuning the ZnPorI 2 to DVB ratio, it is possible to optimize the porosity, morphology, and content of Zn-porphyrin. Owing to the synergistic effect of Zn 2+ and I − , the as-prepared ZnPorI 2 /30DVB exhibited excellent catalytic activities in the cycloaddition of carbon dioxide with epoxides.
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ENERGY & FUELS
·
2024
·
IF 5.2
Shidong Zhou,Yuer Zhao,Xiaoyan Li,Qianli Ma,Hui Du,Xiaofang Lv,Zhilei Wu
The carbon capture and storage technology based on the hydrate method can effectively capture CO2 gas and reduce greenhouse gas emissions; however, the slow and random formation of hydrate has greatly hindered the commercial application of this technology. The effect of l-tryptophan (l-trp) on the kinetics of CO2 hydrate formation with graphene oxide (GO) was investigated. The results showed that the combination of l-trp and GO could effectively accelerate the hydrate formation rate, increase the gas consumption, and promote the formation of the CO2 hydrate. Compared with pure water, the optimal concentration of 0.200 wt % l-trp and 0.020 wt % GO can increase the cumulative gas consumption by 16.229%, shorten the induction time by 69.300%, and shorten the time of 90% hydrate formation by 54.895%. Kinetic experiments and morphological observations show that a low dose of GO could promote heat and mass transfer in the process of CO2 hydrate formation, but with the increase of concentration, GO particles will agglomerate, and the probability of hydrate nucleation will be greatly reduced. The strong wall-climbing effect of l-trp could promote hydrate growth against the reactor wall and gas–liquid exchange. This work provides an experimental basis for the commercialization of the hydrate technology.
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Nano Research
·
2024
·
IF 9.5
Dong Tian,Li Hongdong,Wang Zhenhui,Geng Yanling,Chang Rui,Tian Xiaofeng,Lai Jianping,Feng Shouhua,Wang Lei
Electrocatalytic CO 2 reduction reaction (CO 2 RR) in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral electrolytes. However, the proton-rich environment near the catalyst surface favors hydrogen evolution reactions (HER), leading to lower energy efficiency of the desired products, especially in industrial-level current densities. Here, quaternary ammonium cationic surfactant (cetyltrimethylammonium bromide (CTAB)) was introduced into acidic electrolyte to modulate the interfacial microenvironment, which greatly enhanced CO 2 electroreduction to formic acid (HCOOH) at the Bi/C nanoparticles electrode. Using a Bi/C nanoparticles electrode with CTAB added, constant production of formic acid was enabled with a cathodic energy efficiency of > 40% and maximum FE HCOOH (FE = Faradaic efficiency) of 86.2% at −400 mA·cm −2 over 24 h. Combined with in-situ attenuated total reflection Fourier transform infrared spectroscopy, the concentration of *OCHO intermediates significantly increased after CTAB modification, confirming that the hydrophobic interface microenvironment formed by dynamic adsorption of positively charged long alkyl chains on Bi/C nanoparticle electrodes inhibited HER and improved the selectivity of CO 2 RR to HCOOH.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Minjun Zhou,Zhihao Guo,Mingwang Wang,Dewen Song,Rui Zhou,Hongbin Wang,Shuai Wang,Boshi Zheng,Xiaoshan Wang,Hui Ning,Mingbo Wu
Carbon dioxide electroreduction is a green technology for artificial carbon sequestration, which is being delayed from industrialization due to the lack of efficient catalysts at high current conditions. Herein, the Bi 2 O 3 nanoflakes were uniformly grown on a defective porous carbon (PC). This self-assembling Bi 2 O 3 /PC catalyst was applied to drive CO 2 electroreduction at 1.0 A, 1.5 A and 2.0 A while the Faradaic efficiency of formate reaches 91.50 %, 86.30 % and 84.22 %, respectively. Density functional theory calculations revealed the intrinsic defect of carbon is able to give electron to Bi through O bridge, which increased the electron aggregation of Bi and lowered the generation energy barrier of *OCHO intermediate. Additionally, the unique 3D network of staggered Bi 2 O 3 enhances the CO 2 adsorption and favors the electron transportation. By integrating all above advantages into a solid electrolyte-type cell, we are able to produce pure formic acid in a rate of 15.48 mmol h −1 at ampere current.
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