ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Chengqi Guo,Enhui Jiang,Qiuli Chen,Wanhe Li,Yahui Chen,Shuhan Jia,Yiying Zhou,Zhonghuan Liu,Xinyu Lin,Pengwei Huo,Chunxiang Li,Yun Hau Ng,John Charles Crittenden,Zhi Zhu,Yan Yan
Efficient photocatalytic solar CO2 reduction presents a challenge because visible-to-near-infrared (NIR) low-energy photons account for over 50% of solar energy. Consequently, they are unable to instigate the high-energy reaction necessary for dissociating C═O bonds in CO2. In this study, we present a novel methodology leveraging the often-underutilized photo-to-thermal (PTT) conversion. Our unique two-dimensional (2D) carbon layer-embedded Mo2C (Mo2C–Cx) MXene catalyst in black color showcases superior near-infrared (NIR) light absorption. This enables the efficient utilization of low-energy photons via the PTT conversion mechanism, thereby dramatically enhancing the rate of CO2 photoreduction. Under concentrated sunlight, the optimal Mo2C–C0.5 catalyst achieves CO2 reduction reaction rates of 12000–15000 μmol·g–1·h–1 to CO and 1000–3200 μmol·g–1·h–1 to CH4. Notably, the catalyst delivers solar-to-carbon fuel (STF) conversion efficiencies between 0.0108% to 0.0143% and the STFavg = 0.0123%, the highest recorded values under natural sunlight conditions. This innovative approach accentuates the exploitation of low-frequency, low-energy photons for the enhancement of photocatalytic CO2 reduction.
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Gas Science and Engineering
·
2024
·
IF 0
Xuebi Du,Dawei Shao,Yinhua Wan
Metal-organic frameworks (MOFs) have shown potential as nanofillers for the selective capture of specific gases in mixed matrix membranes (MMMs). This study introduces an efficient method, utilizing a mild (100 °C) reaction condition and a short reaction time (20 min), for the synthesis of MOF-808(Ce) nanocrystals. The MOF-808(Ce) that is obtained exhibits porous characteristics, a notable affinity for CO 2 , and robust intermolecular interactions with PIM-1. Furthermore, this study pioneers the incorporation of MOF-808(Ce) as a filler into PIM-1, with varying loadings, to create PIM/MOF-808 MMMs for the purpose of CO 2 separation. Consequently, the MMMs containing 2 wt% MOF-808(Ce) demonstrate high CO 2 permeability of 6854 Barrer and CO 2 /N 2 selectivity of 23.2, which is far surpasses 2008 upper bound from Robeson and approaches the refined 2019 upper bound from MeKenow. A comparative analysis demonstrates the efficacy of MOF-808(Ce) as a filler in PIM-1 for the purpose of CO 2 separation.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Zhai Jianxin,Xia Zhanghui,Zhou Baowen,Wu Haihong,Xue Teng,Chen Xiao,Jiao Jiapeng,Jia Shuaiqiang,He Mingyuan,Han Buxing
Upcycling of CO 2 into fuels by virtually unlimited solar energy provides an ultimate solution for addressing the substantial challenges of energy crisis and climate change. In this work, we report an efficient nanostructured Ru/MnO x catalyst composed of well-defined Ru/MnO/Mn 3 O 4 for photo-thermal catalytic CO 2 hydrogenation to CH 4 , which is the result of a combination of external heating and irradiation. Remarkably, under relatively mild conditions of 200 °C, a considerable CH 4 production rate of 166.7 mmol g −1 h −1 was achieved with a superior selectivity of 99.5% at CO 2 conversion of 66.8%. The correlative spectroscopic and theoretical investigations suggest that the yield of CH 4 is enhanced by coordinating photon energy with thermal energy to reduce the activation energy of reaction and promote formation of key intermediate COOH* species over the catalyst. This work opens up a new strategy for CO 2 hydrogenation toward CH 4 .
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FUEL
·
2024
·
IF 6.7
Yiming Chen,Chuan Wang,Qianwen Zhang,Ling Zhou,Yi Zhang
Methane synthesis derived from CO 2 hydrogenation has attracted great attention in terms of CO 2 recycling while suffering from the loss and sintering of active nickel species. Hence, we synthesized the Ni@Beta (Si/Al = 40) catalyst with a specific encapsulated structure by a simple hydrothermal synthesis using conventional Ni/SiO 2 as a unique silicon source. Compared to the conventional Ni/SiO 2 and Ni/Al 2 O 3 , the Ni@Silicalite-1 and Ni@Beta with encapsulated structures showed better stability. In addition, the Ni@Beta simultaneously exhibited the highest CO 2 conversion (74.2 %) and methane selectivity (93.5 %). All obtained catalysts were characterized by BET, ICP- OES, XRD, SEM-EDS, HRTEM, H 2 -TPR, CO 2 -TPD, in situ XPS, in situ DRIFTS, and NAP-XPS. Compared with the Ni@Silicalite-1 (Al-free zeolite), the aluminum-containing zeolite frameworks of the Ni@Beta got more electrons from the nickel active phases, so the metal-support interaction on the Ni@Beta was stronger, which was favorable for the stability of the Ni 0 phase. In addition, the Al-containing zeolite frameworks of the Ni@Beta inhibited the formation of volatile metal–molecule intermediates (gaseous Ni(CO) x ), which prevented serious sintering and loss of the nickel species. The in situ DRIFTS and NAP-XPS results not only successfully unveiled that the main reaction pathway was a formate route, but also showed that the Ni@Beta had the strongest capacity to adsorb and convert CO 2 , so it had the highest methanation activity.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2025
·Vol. 51
·期 4
·2071-2088
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IF 3.5
Wu Yilin,Li Yiping,Zhang Kai,Hu Jinhai,Yan Hong
Photocatalytic CO 2 reduction technology can use sunlight to convert CO 2 into fuel or chemical raw materials, slowdown the greenhouse effect and achieve sustainable development. Therefore, we have developed a series of high-quality carbon quantum dots using alkaline lignin (AL) as the core raw material and using high efficiency hydrothermal method. Ag-BiVO 4 composite was prepared by hydrothermal method. Then, the Ag-BiVO 4 -CQDs photocatalytic composite was prepared by constant temperature water bath method. The structure and morphology of the composites were characterized by X-ray diffraction, transmission electron microscope and X-ray photoelectron spectroscopy. Through optical and electrochemical tests, it can be seen that the composite has better interfacial charge transfer and electron transport ability. In the visible light catalytic CO 2 reduction reaction, Ag-BiVO 4 can selectively reduce CO 2 to CH 4 , and the CH 4 yield is greatly improved after Ag-BiVO 4 combines with CQDs. The 3 h CH 4 yield increased from 17.64 μmol/g to 97.82 μmol/g after reduction by adding 40 mL CQDs to Ag-BiVO 4 composite, which is 5.54 times that of Ag-BiVO 4 . The results showed that the introduced CQDs were uniformly attached to Ag-BiVO 4 . As an electron transport medium, CQDs can efficiently facilitate the transfer of photogenerated carriers, suppress the recombination of electron–hole pairs, and enhance the photocatalytic performance of Ag-BiVO 4 -CQDs for CO 2 reduction.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Zhongcheng Yang,Yue Yang,Yunna Li,Junwen Qi,Zhigao Zhu,Yujun Zhou,Jiansheng Li
A novel hollow fiber membrane containing a carbon-coated CuO x (CuC-HFM) was prepared for in-situ CO 2 electrochemical reduction to ethanol during wastewater treatment. The ratio of Cu-based metal organic framework/carbon black of 1/1 was relatively optimal (Cu 1 C 1 -HFM) due to higher pure water permeance (24.62 L m −2 h −1 bar −1 ), better hydrophilicity (contact angle of 60.00°), and more ethanol yield (165.22 mg L −1 m −1 ) at −2.5 V with KOH as electrolyte. For control group (Cu 2 C 1 -HFM and Cu 1 C 2 -HFM), they were 76.50°/89.10°, 3.90/4.42 L m −2 h −1 bar −1 , 64.85/57.32 mg L −1 m −1 , respectively. The peaks of Cu (002) crystal plane, Cu 2+ electronic orbits, covalent bonds between C and O, and CuO x were appeared on prepared membrane. The CuO x could strongly adsorb CO and subsequently carbon shell could selectively produce HOCCH and HOCHCH, which were benefit for CO 2 electro reduction to ethanol. Therefore, the Cu 1 C 1 -HFM owned higher ethanol production (88.50 g L −1 m −2 h −1 ) during filtrating anaerobic supernatant. Meanwhile, the membrane could reject 97.2 % COD with only 14.7 % membrane flux loss. The membrane without bias suffered 27.1 % flux loss. This system gave a new thought for CO 2 electro reduction and the CuC-HFM had a promising employment in anaerobic bioreactor in the future.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Mengchen Wu,Yang Yang,Jing Zhao,Rui Liu
In CO 2 electroreduction, mutative intermediates and the challenging C C coupling necessitate the spatial interplay between active sites and through dynamically optimizing configurations. Herein, we anchor ethylenediaminetetraacetic acid (EDTA)-bonded Cu x+ /Bi 3+ pair within UiO-66 for a spontaneous spatial-optimizing CO 2 -to-C 2 H 4 electroreduction. Ab initio molecular dynamic (AIMD) simulation visualizes that such metal pair adaptively interacts with intermediates. Density functional theory (DFT) elicits the componential synergy, in which an upshift d-band of Cu activates CO 2 being protonated into *COOH while Bi site stabilizes oxygenated dimers for deep hydrogenation. The dynamic feature of such pair affords large freedom for sorption and migration of various intermediates, which consequently bestows UiO-66-EDTA/CuBi a maximal FE C 2 H 4 of 47 % and a total current density over 100 mA cm −2 in the flow cell.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Shichen Zeng,Xu Liang,Mingang Zhao,Yanxiong Ren,Hanze Ma,Ziting Zhu,Yuhan Wang,Shaoyu Wang,Junyi Zhao,Guangzhaoyao Yang,Xuerui Wang,Fusheng Pan,Guangwei He,Zhongyi Jiang
Covalent organic frameworks (COF) are deemed as disruptive membrane materials owing to their versatile functionalities, high stability and ordered nanochannels. However, the size mismatch between the COF intrinsic pore and gas molecules becomes a grand challenge when using COF membrane for carbon capture. Herein, we propose a new type of polymer-functionalized COF laminar membranes through grafting CO 2 -phlic polyethyleneimine (PEI) polymer onto carboxylic acid COF (cCOF) laminar membranes. The cCOF nanosheets with high density of carboxyl groups are prepared via modified single phase solution method and then assembled to fabricate membranes. Further, the cCOF membranes are functionalized with PEI using 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide/N-Hydroxysuccinimide (EDC/NHS) coupling chemistry. The introduction of abundant amino groups from PEI afford the affinity of membranes toward CO 2 . Meanwhile, the graft of the PEI polymers reduces the defects or pinholes on the membrane surface. As a result, the PEI functionalized cCOF membranes exhibit a high CO 2 permeance of 1004 GPU and a CO 2 /N 2 selectivity of 33.7, which reach the carbon capture target performance and show great prospect for treating real flue gas. Our approach of functionalizing cCOF membranes with tailored functionalities may inspire the design of molecule-selective COF membranes.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xiao-Han Li,Bo-Wen Zhang,Wan-Feng Xiong,Ze Li,Xiao-Yu Xiang,Si-Ying Zhang,Duan-Hui Si,Hong-Fang Li,Rong Cao
Electrochemical reduction of carbon dioxide (CO 2 RR) is a promising approach to complete the carbon cycle and potentially convert CO 2 into valuable chemicals and fuels. Cu is unique among transition metals in its ability to catalyze the CO 2 RR and produce multi-carbon products. However, achieving high selectivity for C 2+ products is challenging for copper-based catalysts, as C–C coupling reactions proceed slowly. Herein, a surface modification strategy involving grafting long alkyl chains onto copper nanowires (Cu NWs) has been proposed to regulate the electronic structure of Cu surface, which facilitates *CO-*CO coupling in the CO 2 RR. The hydrophobicity of the catalysts increases greatly after the introduction of long alkyl chains, therefore the hydrogen evolution reaction (HER) has been inhibited effectively. Such surface modification approach proves to be highly efficient and universal, with the Faradaic efficiency (FE) of C 2 H 4 up to 53% for the optimized Cu–SH catalyst, representing a significant enhancement compared to the pristine Cu NWs (30%). In-situ characterizations and theoretical calculations demonstrate that the different terminal groups of the grafted octadecyl chains can effectively regulate the charge density of Cu NWs interface and change the adsorption configuration of *CO intermediate. The top-adsorbed *CO intermediates (*CO top ) on Cu–SH catalytic interface endow Cu–SH with the highest charge density, which effectively lowers the reaction energy barrier for *CO-*CO coupling, promoting the formation of the *OCCO intermediate, thereby enhancing the selectivity towards C 2 H 4 . This study provides a promising method for designing efficient Cu-based catalysts with high catalytic activity and selectivity towards C 2 H 4 .
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Deng Xianyu,Zhang Jianjun,Qi Kezhen,Liang Guijie,Xu Feiyan,Yu Jiaguo
Constructing S-scheme heterojunctions proves proficient in achieving the spatial separation of potent photogenerated charge carriers for their participation in photoreactions. Nonetheless, the restricted contact areas between two phases within S-scheme heterostructures lead to inefficient interfacial charge transport, resulting in low photocatalytic efficiency from a kinetic perspective. Here, In 2 O 3 /Nb 2 O 5 S-scheme heterojunctions are fabricated through a straightforward one-step electrospinning technique, enabling intimate contact between the two phases and thereby fostering ultrafast interfacial electron transfer (<10 ps), as analyzed via femtosecond transient absorption spectroscopy. As a result, powerful photo-electrons and holes accumulate in the Nb 2 O 5 conduction band and In 2 O 3 valence band, respectively, exhibiting extended long lifetimes and facilitating their involvement in subsequent photoreactions. Combined with the efficient chemisorption and activation of stable CO 2 on the Nb 2 O 5 , the resulting In 2 O 3 /Nb 2 O 5 hybrid nanofibers demonstrate improved photocatalytic performance for CO 2 conversion.
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LANGMUIR
·
2024
·
IF 3.7
Zhuoxue Li,Yunlei Shi,Yimian Ding,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Jikuan Qiu,Xiaopeng Xuan,Jianji Wang
A Pickering emulsion is a natural microreactor for interfacial catalysis in which an emulsifier is critical. Recently, a metal–organic framework (MOF) has attracted attention to emulsify water–organic mixtures for constructing a Pickering emulsion. However, a few stimuli-responsive Pickering emulsions based on MOFs have been reported, and the MOF emulsifiers cannot be regenerated at room temperature. Herein, the Zr-MOF with a rodlike morphology is synthesized using ionic liquid as a modulator and then modified with n-(trimethoxysilylpropyl)imidazole (C3im) to prepare a series of functionalized Zr-MOFs (MOF-C3im). It is found that MOF-C3im is an excellent emulsifier to construct stable and CO2-responsive Pickering emulsions even at low content (>0.20 wt %). Notably, the emulsification and demulsification of the emulsions can be easily and reversibly switched by bubbling of CO2 and N2 alternatively at room temperature because CO2 and imidazole molecules anchored on the Zr-MOF underwent a reversible acid–base reaction, resulting in an obvious change in the wettability of the emulsifier. As a proof of concept, the reduction reactions of nitrobenzene have been successfully carried out in these Pickering emulsions, demonstrating the efficient integration as a microreactor for chemical reaction, product separation, and emulsifier recycling under ambient conditions. This strategy provides an innovative option to develop stimulus-responsive Pickering emulsions for sustainable chemical processes.
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Energy Technology
·
2024
·
IF 3.6
Xueli Zhang,Shan Hu,Fangyuan Zhang,Shuchen Xing,Huilin Hu,Jinhua Ye,Defa Wang
As a promising technology to mitigate global carbon emissions, photothermal catalytic CO 2 reduction remains a great challenge in increasing the conversion efficiency and regulating the product selectivity. Herein, a series of phase-separated Ni–Mo alloy catalysts for efficient photothermal CO 2 reduction with tunable CO selectivity is reported. With the increase of Mo content, the evolution rate and selectivity of CO increases. The optimal catalyst Ni 1 Mo 1 achieves 32.1% CO 2 conversion with 98.0% of CO selectivity and 71.1 mmol g cat −1 h −1 of CO evolution rate under a 300 W xenon lamp irradiation. Further increasing the Mo content reduces the CO evolution rate while maintaining the high CO selectivity. In the mechanistic study, it is revealed that the Ni–Mo alloy with an appropriate Ni/Mo ratio (e.g., Ni 1 Mo 1 ) possesses a modified electronic structure with more negative d-band center, which increases the light absorption, reduces the H 2 dissociation, and favors the CO desorption, thereby leading to efficient and selective photothermal reduction of CO 2 to CO. In this work, a viable strategy to design nickel-based catalysts is provided for efficient and selective photothermal CO 2 reduction via composition-mediated modification of electronic structure.
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