Sustainable Energy & Fuels
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2025
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IF 4.1
Yongheng Xiong,Yang Yu,Huangang Shi,Jifa Qu,Wenyi Tan
Single atom Fe sites, doped in CN materials, exhibit outstanding electrochemical activity for CO2-to-CO conversion. The pyrolysis of ZIF8 is a controllable method for fabricating isolated single atom metal sites. In this study, we propose a new strategy to increase the ratio of Fe in ZIF8 precursors by synergistically replacing Zn2+ with Bi3+ and Fe3+. After precursor pyrolysis, the obtained Bi/Fe–N–C catalysts, consisting of Bi sites and pyrrole-type Fe–Nx sites, serve as efficient electrocatalysts for the CO2RR. The results show that the optimized catalyst loaded with 94.8 mg per kgCat Fe exhibits a high FECO of >90.1% over a wide potential range of −0.4 to −0.7 VRHE (98.2% at −0.5 VRHE). Insights into the electrochemical reaction mechanism show that this successful design of Bi/Fe–N–C catalysts can provide a stable catalytic site to form *COOH, thus achieving energy-efficient electrochemical CO2 reduction to CO.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2025
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IF 3.7
Yongxian Liu,Zhihua Feng,Zhangting Dang,Qingqing Hou,Yue Yu,Xiaofei Zhao,Lingling Wang,Yong He,Renbo Wei,Xiufu Hua
Converting CO 2 efficiently into high-value-added chemical products represents dual value in ecological conservation and resource valorization. Designing novel catalysts integrating atom economy and process intensification constitutes the cornerstone for catalytic CO 2 conversion. Herein, an integrated polymeric heterogeneous catalyst is constructed by covalently anchoring functional groups of quaternary ammonium (QA) and copper phthalocyanine (CuPc) onto a polyurea (PU) framework, yielding PU-CuPc-QA. This catalyst is subsequently applied for CO 2 conversion to cyclic carbonates. Owing to the Cu 2+ centers in phthalocyanine and urea groups from PU acting as a Lewis acid and hydrogen bond donor (HBD) to efficiently activate epoxide, as well as nucleophilic attack of this activated epoxide by iodide ion (I - ) dissociated from QA, PU-CuPc-QA facilitates ring-opening of epoxide. Moreover, the phthalocyanine rins and the QA cations in PU-CuPc-QA work as N -rich groups that can adsorb and active CO 2 . As a result, PU-CuPc-QA exhibits exceptional catalytic activity for CO 2 cycloaddition under mild conditions without adding any external co-catalysts. Specially, at 100 o C, 1.5 MPa of CO 2 , 6%(mass) PU-CuPc-QA achieve 99% propylene carbonate yield and selectivity after reacting with propylene oxide for 6 h. Combining its ability to catalyze and activate epoxide and CO 2 simultaneously, PU-CuPc-QA is a promising catalyst for CO 2 cycloaddition.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Meisi Chen,Dandan Hao,Yuwen Shao,Tong Zhao,Chengyi Qiu,Xiemin Liu,Muhua Chen,Gang Zhang,Xinbao Zhu,Bo Fu
Cellulose directs Mg/Ni-MOF-74 growth on fiber surfaces. • Tuning Mg/Ni ratio optimizes pore structure and open metal site characteristics. • MNC-1 exhibits high CO 2 capacity and CO 2 /N 2 selectivity (>200). • Hierarchical porosity facilitates both CO 2 confinement and gas mass transfer. • Low isosteric heat of adsorption promotes easy regeneration. To overcome the poor dispersibility and limited gas mass transfer of MOF powders, a series of Mg/Ni-MOF-74/cellulose composites (MNC-x) were fabricated via cellulose interface directed in situ growth. The effects of the Mg/Ni ratio on the material structure and CO 2 /N 2 adsorption performance were investigated. Results showed that the introduction of Ni altered the local environment and crystal size, regulating the pore structure and adsorption sites of the MNC-x series materials. The optimal sample (MNC-1) achieved a static CO 2 adsorption capacity of 2.67 mmol·g −1 at 298 K and exhibiting superior cycling performance. IAST theoretical calculations indicated that MNC-1 possessed high CO 2 /N 2 selectivity, with an initial isosteric heat of adsorption of only 34.51 kJ·mol −1 , indicating that physical adsorption was predominant. Combined with DFT analysis, the excellent CO 2 adsorption performance of MNC-1 was mainly attributed to the interaction between the open metal sites of Mg/Ni and CO 2 , as well as the hierarchical pore structure formed by the microporous adsorption sites and mesoporous mass transfer channels. This study provides a feasible strategy for designing cellulose-supported, processable bimetallic MOF adsorbents for CO 2 adsorption. Download: Download high-res image (269KB) Download: Download full-size image
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Chengli Jiao,Zedong Li,Xinxin Li,Mian Wu,Heqing Jiang
Poor interfacial compatibility that often led to low gas separation performance is one of key challenges for developing composite membranes. In the present study, nanosized polyethyleneimine (PEI) functionalized ZIF-8 (PEI-ZIF-8) with good dispersion, having a particle size around 15 nm, has been synthesized via in-situ method and used as filler to fabricate Pebax/PEI-ZIF-8 composite membranes. Excluding the intrinsic porous structure and higher affinity with CO 2 of PEI-ZIF-8 beneficial for CO 2 selective transport, the large density of amine groups on PEI chains provide a good interfacial compatibility, and introduce facilitated CO 2 transport path. Furthermore, PEI-ZIF-8 reduces the crystallinity of Pebax matrix, which is favorable for CO 2 transport. The composite membrane with 5 wt% PEI-ZIF-8 shows a CO 2 permeance of 13.0 GPU with a CO 2 /N 2 selectivity of 49.0, which increases by 80.6% and 118.8% respectively in contrast with pristine Pebax membrane. The results demonstrate that nanoparticles functionalized by amine-polymer with long chains is effective for constructing composite membranes with good interfacial compatibility.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2016
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IF 2.628
Li Liu,Na Tian,Long Huang,Yu-Hao Hong,Ai-Yun Xie,Feng-Yang Zhang,Chi Xiao,Zhi-You Zhou,Shi-Gang Sun
The modification of oxide-derived Cu electrode with Ni, Zn, and Au was examined to improve the catalytic activity of CO 2 electroreduction. The experimental results showed that Ni modification increased the Faraday efficiency of the formation of formic acid and n -propanol. The Faraday efficiency relating to the formation of the liquid products was as high as 34.3% at −1.5 V versus the saturated calomel electrode reference potential. In contrast, modification with Zn reduced the formic acid formation efficiency but enhanced the alcohol formation efficiency. Finally, modification with Au suppressed the selectivity toward the formation of both formic acid and alcohols.
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DOI
高影响因子
NEW CARBON MATERIALS
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2022
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IF 3.7
Hong-zhi Wang,Yue-zhu Zhao,Zhong-xue Yang,Xin-ze Bi,Zhao-liang Wang,Ming-bo Wu
Using CO 2 as a renewable carbon source for the production of high-value-added fuels and chemicals has recently received global attention. The photoelectrocatalytic (PEC) CO 2 reduction reaction (CO 2 RR) is one of the most realistic and attractive ways of achieving this, and can be realized effectively under sunlight illumination at a low overpotential. Oxygen-incorporated carbon nitride porous nanosheets (CNs) were synthesized from urea or melamine by annealing in nitrogen or N 2 /O 2 gas mixtures. They were used as the photoanode with Bi 2 CuO 4 as the photocathode to realize PEC CO 2 reduction to the formate. The electrical conductivity and the photoelectric response of the CNs were modified by changing the oxygen source. Oxygen in CNs obtained from an oxygen-containing precursor improved the conductivity because of its greater electronegativity, whereas oxygen in CNs obtained from the calcination atmosphere had a lower photoelectric response due to a down shift of the energy band structure. The CN prepared by annealing urea, which served as the source of oxygen and nitrogen, at 550 °C for 2 h in nitrogen is the best. It has a photocurrent density of 587 μA cm −2 and an activity of PEC CO 2 reduction to the formate of 273.56 μmol cm −2 h −1 , which is nearly 19 times higher than a conventional sample. The CN sample shows excellent stability with the photocurrent remaining constant for 24 h. This work provides a new way to achieve efficient catalysts for PEC CO 2 reduction to the formate, which may be expanded to different PEC reactions using different cathode catalysts.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2019
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IF 4.182
Miao Zhang,Ruijin Zheng,Ying Ma,Ruiping Chen,Xun Sun,Xuan Sun
Three 2D N-rich COFs linked by –C=N– bond, named COF-SDU1, COF-SDU2, COF-SDU3, have been synthesized via the Schiff-base condensation reaction . Tri-(4-formacylphenoxy)-1,3,5-triazine (TRIF) is employed as N-rich aldehyde building block, and p-phenylenediamine (PA), hydrazine hydrate, and terephthalic dihydrazide (TPDH) are as the amine building blocks, respectively, which results in high crystallinity, high BET surface area, and abundant N-atom sites for COF-SDU1, COF-SDU2, and COF-SDU3. COF-SDU1 exhibits large CO 2 uptake of 741 mg g −1 at 298 K under 45 bar, while COF-SDU2 is 484 mg g −1 and COF-SDU3 is only 331 mg g −1 , which are closely related to their specific surface area but irrespective of the absolute N-content. The result clearly reveals the impact of various factors, including N-content, BET surface area and pore size on CO 2 storage performance. It shows that N-content determines capacities at low pressure (<1 bar), BET surface area plays the decisive role under relative low pressure (<25 bar) and large pore size helps enhance the capacity under relative high pressure (>25 bar). Among all factors, BET surface area plays the crucial role in determining the high-pressure CO 2 storage capacity, which is well verified by theoretical modeling.
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高影响因子
CATALYSIS TODAY
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2024
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IF 5.2
Yanan Jiang,Huayu Sun,Yuzhen Fang,Cuijuan Zhang,Yuan Liu
The sintering issue of Ni nanoparticles seriously limits the practical application of the Ni-based catalysts for CO 2 methanation. This work demonstrates that the La- and Ce- dual-promoted Ni/ZrO 2 shows better durability at 600 ºC and 60000 mL g cat −1 h −1 over 200 h compared with the La- or Ce- single-promoted. The composition and microstructure characterization indicates that the dispersion and sintering resistance of Ni nanoparticles is enhanced with the dual-promoted catalysts. Both depth profile of X-ray photoelectron spectroscopy and density functional theory calculation show that in the La- and Ce- dual-promoted Ni/ZrO 2 , the reduced dissolution of Ce into ZrO 2 lattice and the spread of La on ZrO 2 surface by forming a La 2 O 3 -CeO 2 solid solution improves the dispersion and stability of Ni nanoparticles. This work provides a facile strategy to mitigate the sintering of Ni nanoparticles and thus improve the stability of Ni-based catalysts for CO 2 methanation.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Huihui Ding,Huanhuan Wu,Jun Ma,Xiang Li,Shuangshuang Huai,Chengming Zhang,Haibao Zhu,Ping Li,Jie Li,Xiufang Wang,Wenjie Xie
Artificial photosynthesis converting CO 2 into valuable compounds has garnered significant interest. However, the insufficient surface activity sites, weak adsorption capacity of CO 2 and poor electron-hole separation capability hinder CO 2 photoreduction used for practical implementation. Herein, Bi nanoparticles/Bi 24 O 31 Br 10 composite photocatalyst (Bi/BOB) was designed constructed through in-situ reduction of bismuth metal on the surface of ultra-thin Bi 24 O 31 Br 10 nanosheets. Bi/BOB exhibits an excellent ability to reduce CO 2 to CO. The CO 2 reduction rate of the optimized Bi/BOB composite catalyst is 43.07 μmol·g −1 ·h −1 , which is significantly superior to other reported bismuth-based photocatalysts. Experimental characterization and Theoretical simulation calculation reveal that the in-situ reduction of bismuth metal causes significant local lattice distortion and uneven charge distribution, thereby producing a strong interaction between Bi nanoparticles and BOB support. So, it enhances the adsorption and activation of carbon dioxide molecules and reduces the Gibbs free energy barrier during the catalytic reaction. Moreover, the strong interaction helps to enhance the separation of photogenerated charge carriers and stability of catalysts. This study offers research suggestions for the interaction between metal and support to enhance CO 2 reduction.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Lingyu Shao,Feng Xu,Zhicheng Wu,Chang Liu,Chengjin Pan,Yifan Wang,Zhengda Yang,Tao Wang,Longchao Yao,Chenghang Zheng,Xiang Gao
Advancement of the absorbent for CO 2 capture is essential in optimizing the performance and reducing the negative environmental effects associated with this technology. Despite ammonia's promise as an absorbent, the volatility limits its practical application and creates potential environmental pollution . Therein, we assess various additives (amino acids, carbonates, and alkanolamines) for ammonia-based solvents using multi-stage circulation absorber from the viewpoints of aerosol emission, ammonia emission, and CO 2 capture efficiency. Experimental findings reveal that ammonia volatilization can be inhibited by the protonation of free ammonia by carboxyl groups and the formation of hydrogen bonding between amino/hydroxyl groups and ammonia, with ammonia emission reduced by 21.7 %, aerosol emission reduced by 26.5 %, and CO 2 capture efficiency increased to a maximum of 87.8 % under the condition of adding histidine . Moreover, the experiment highlights a positive correlation between total ammonia emission and aerosol concentration/diameter. Additionally, tests combining source abatement with water wash exhibit up to 50.5 % aerosol removal efficiency and up to 76.6 % ammonia removal efficiency. To further mitigate emissions, a comprehensive approach is proposed, achieving an 84.4 % reduction in ammonia emission and a 61.9 % reduction in aerosol emission. Finally, a method for recycling ammonia for desulfurization is suggested.
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Jiayue Yu,Yang Zheng,Binxin Lv,Aiming Huang,Junjun Zhang,Zizi Wang,Yifan Zhang,Yang Wu,Yanan Zhou,Yong Wang,Wen Luo
Covalent organic frameworks (COFs), with their unique structures, have gained attention in CO 2 reduction (CO 2 RR) and are often combined with metal active sites to enhance performance. However, the weak interactions between COFs and metals create ambiguity about their actual states under reaction conditions, hindering the design of high-performance catalysts. Understanding these interactions is therefore essential for the rational development of advanced CO 2 RR electrocatalysts. Herein, a TpBpy COF, synthesized from 2,4,6-triformylphloroglucinol (Tp) and 5,5′-diamino-2,2′-bipyridine (Bpy), was coordinated with copper acetate to serve as a model catalytic system for understanding the structural evolution of TpBpy-Cu during CO 2 RR and the corresponding impact on the catalytic performance. A selectivity shift from CO to multi-carbon products was observed with increasing Cu content and reaction time. By combining ex situ characterization techniques with in situ infrared and Raman spectroscopy, the reduction of TpBpy-Cu to metallic Cu particles was revealed. Density functional theory calculations further demonstrated that metallic Cu surfaces of the resulting Cu particles played a key role in lowering the C-C coupling free energy change, facilitating the production of multi-carbon products. This work provides fundamental insights into the application of copper-based COF composite catalysts in electrocatalytic CO 2 RR and offers valuable guidance for the design of more efficient Cu-COF composite catalysts.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Meng Linghu,Yang Jiakun,Huo Zichen,Wu Qin,Zhang Yaoyuan,Shi Daxin,Chen Kangcheng,Liu Helei,Xu Xiyan,Li Hansheng,Xu Hang
The capture and transformation of CO 2 , utilized as a C1 resource, play an integral role in mitigating CO 2 emissions and addressing the emerging 'carbon source crisis.' The CO 2 cycloaddition to cyclic carbonate is particularly noteworthy. A critical factor in optimizing the efficiency and minimizing the costs associated with CO 2 cycloaddition is the selection of an effective catalyst. A novel amine-functionalized intramolecular acid-base synergistic ZIF catalyst, designated as ABF-ZIF-X, was synthesized using a mixed ligand method, employing 2-MeIM and the larger molecular-sized ligand 2-amBzIM. The introduction of an amino active center and the strategic regulation of the active site defects in metal ions enable ABF-ZIF-X to enhance the density of Lewis acid and base sites. This enhancement facilitates intramolecular acid-base cooperation, which is pivotal for effective CO 2 cycloaddition catalysis. Notably, ABF-ZIF-X exhibits exceptional catalytic activity in the cycloaddition of EBH with CO 2 , eliminating the need for additional solvents and co-catalysts. The reaction mechanism of CO 2 cycloaddition, which is intramolecular acid-base synergistic catalysis and bimolecular activation, was proposed. Among the synthesized catalysts. ABF-ZIF-0.15 shows superior performance, achieving an impressive 96.7% conversion of EBH and a selectivity of 97.1%. Furthermore, this catalyst demonstrates remarkable reusability, maintaining high activity across five cycles.
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高影响因子
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