Carbon Neutrality
·
2024
·Vol. 3
·期 1
·1-20
·
IF 0
Guo Yafei,Gao Yuxuan,Guo Benshuai,Luo Yangna,Zhao Guoyang,Sun Jian,Li Weiling,Wang Ruilin,Zhao Chuanwen
Electrochemical CO 2 reduction (ECR) to value-added products is regarded as a sustainable strategy to mitigate global warming and energy crisis, and designing highly efficient and robust catalysts is essential. In this work, transition metal sulfides (TMS)-decorated CuS microflower-like structures were prepared via the one-pot hydrothermal synthesis method for ECR to CO, and the influence of TMS doping on ECR performance was demonstrated. Characterization of the catalysts was performed using XRD, FESEM-EDS, N 2 physisorption, and XPS, revealing the successful loading of TMS, the formation of microflower-like architectures and the generation of sulfur vacancies. Electrochemical tests demonstrated that doping ZnS, Bi 2 S 3 , CdS and MoS 2 improved the intrinsic CO 2 reduction activity of the CuS catalyst. Particularly, the MoS 2 -CuS composite catalyst with imperfect petal-like structure showed uniform distribution of edge Mo sites, which worked synergistically with the formed grain boundaries (GBs) and undercoordinated S vacancy sites in promoting CO 2 activation, stabilizing * COOH adsorption, facilitating * CO desorption, and lowering the energy barrier of the potential-limiting step for improved CO selectivity. The MoS 2 -CuS catalyst achieved a maximum CO selectivity of 83.2% at –0.6 V versus the reversible hydrogen electrode (RHE) and a high CO cathodic energetic efficiency of 100%. At this potential, the catalyst maintained stable catalytic activity and CO selectivity during a 333-min electrolysis process. The findings will offer a promising avenue for the development of efficient and stable catalysts for CO production from ECR.
研究领域:
材料科学
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环境科学
·
能源化学
✓ 已验证
DOI
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Bingchen Chen,Chao Wan,Xueting Kang,Mingqing Chen,Chunfang Zhang,Yunxiang Bai,Liangliang Dong
In this study, a facile and scalable in situ growth method was used to synthesize ZIF-8@GO composites. The obtained ZIF-8@GO were blended with a CO 2 -philic, comb copolymer yielding a series of mixed matrix membranes (MMMs), which were evaluated for their performance in separation of CO 2 /N 2 . The effect of reaction time for ZIF-8@GO composites on gas separation performance was systematically investigated. Pure and mixture gas permeation tests indicated that MMM with ZIF-8@GO by in situ growth for 6 h exhibited the largest improvement (CO 2 permeability: 475 Barrer and CO 2 /N 2 selectivity: 58.2) compared with pure polymers, with the overall CO 2 /N 2 separation performance exceeding the 2008 polymer upper bound. Our strategy that the in situ growth of ZIF-8 on GO provides an effective way to design MMMs with well filler dispersion, structural features and separation performance.
研究领域:
材料科学
·
环境工程
✓ 已验证
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2021
·Vol. 23
·期 8
·4690-4699
·
IF 3.676
Zhengyan Zhao,Wei Liu,Yantao Shi,Heming Zhang,Xuedan Song,Wenzhe Shang,Ce Hao
We report a combination of experimental and computational mechanistic studies for the photoreduction of CO2 to CO with water, catalyzed by single-atom Fe supported on graphitic carbon nitride (g-C3N4). Density functional theory (DFT) and time-dependent DFT (TDDFT) methods were utilized to explore the behavior of single-atom Fe in g-C3N4, which is of vital importance to the understanding of the CO2 reduction reaction (CO2RR) mechanism. The calculation results reveal that the rate-limiting step of the hydrogen-bonded complex in the absence of Fe atoms is the cleavage of C–O bonds in COOH radicals during the whole CO2RR, which includes the photophysical and photochemical processes. The presence of Fe atoms not only activated CO2 in the ground state and increased the rate constant of the limiting step in the photophysical process, but also functioned as the catalytic active center, lowering the reaction barrier of the C–O bond cleavage in COOH˙ in the photochemical process and resulting in improved photocatalytic activity. In addition, DFT calculations further demonstrated that the electron and proton transfer involved in the photophysical and photochemical processes is closely related to and induced by the hydrogen bonds in the excited state.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
Science Advances
·
2020
·Vol. 6
·期 17
·
IF 13.117
Xiaofei Zhang,Haitao Liu,Pengfei An,Yanan Shi,Jianyu Han,Zhongjie Yang,Chang Long,Jun Guo,Shenlong Zhao,Kun Zhao,Huajie Yin,Lirong Zheng,Binhao Zhang,Xiaoping Liu,Lijuan Zhang,Guodong Li,Zhiyong Tang
CO2 cycloaddition with epoxides at low temperature and pressure has been broadly recognized as an ambitious but challenging goal, which requires the catalysts to have precisely controlled Lewis acid sites. Here, we demonstrate that both stereochemical environment and oxidation state of single cobalt active sites in cobalt tetraaminophthalocyanine [CoPc(NH2)4] are finely tuned via molecular engineering with 2,5-di-tert-butyl-1,4-benzoquinone (DTBBQ). Notably, DTBBQ incorporation not only enables formation of 5-nm-thick conjugated microporous polymer (CMP) nanosheets due to the steric hindrance effect of tert-butyl groups but also makes isolated cobalt sites with high oxidation state due to the presence of delocalized electron-withdrawing effect of alkene groups in DTBBQ via conjugated skeleton. Notably, when used as heterogeneous catalysts for CO2 cycloaddition with different epoxides, single cobalt active sites on the ultrathin CMP nanosheets exhibit unprecedentedly high activity and excellent stability under mild reaction conditions.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2024
·
IF 6.7
Xu Li,Liming Zheng,Guanghui Li,Jingyang Pu,Tong Zhang,Feifei Huang
CO 2 -enhanced oil recovery (CO 2 -EOR) has attracted great attention due to its dual effects of geological carbon storage and economic benefits, but the clay swelling, asphaltene deposition and gas channeling induced by CO 2 still restrict its field application. The employment of chemical agents for the purpose of improving CO 2 -EOR performance is often limited by the heterogeneity of reservoirs and the potential for formation damage. Physical methods, such as ultrasonic-assisted CO 2 flooding, appear to offer a promising alternative for CO 2 -EOR and geological sequestration. This study has conducted oil displacement experiments to investigate the EOR potential of ultrasonic-assisted CO 2 flooding in tight reservoirs and clarify the effects of different ultrasound parameters. The ultrasonic waves with 20 kHz of acoustic frequency, 30 W/cm 2 of sound intensity, 30 min of sonication time and moderate intermittent working mode can yield violent cavitation effects and avoid undesirable energy dissipation. Nearly a quarter of the saturated crude oil can be recovered from the tight core through ultrasonic-assisted CO 2 flooding. It can be attributed to the composition alterations of crude oil and property changes of core matrix. Coupling with ultrasonic waves, CO 2 would extract and vaporize crude oil more easily, which promotes oil swelling, lowers oil density and viscosity, decreases oil–gas interfacial tension and thus improves oil recovery. Besides, the ultrasound can help to mitigate the impact of CO 2 adsorption-induced clay swelling on pore sizes through fluctuating pressure. And the strong hydrodynamic shear forces generated by mechanical vibration of ultrasound may also help to connect individual small pores and extend micro-fractures. These synergistic effects result in the transformation of micropores into mesopores and macropores. Furthermore, the wettability alteration of core samples implies that the ultrasonic-assisted CO 2 flooding can induce the detachment of oil films from the rock surface. Finally, the results of molecular dynamics simulations indicate that the improvement in pressure inside the core sample resulting from ultrasonic cavitation facilitates the mixing of CO 2 and oil, thereby weakening gas channeling and improving the displacement efficiency.
研究领域:
石油工程
·
地质学
·
物理化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ya-Nan Jing,Xing-Liang Yin,Lei-Lei Li,Yan-Lan Wang,Jia Xue,Ze-Feng Xu,Da-Qiang Liu,Chuan-Wu Chen,Xiao-Jie Liu,Er-Kang Liu
CO 2 -to-high value-added chemicals via a photocatalytic route is of interest but strangled by the low efficiency. Herein, a novel Fe-TiO 2-x /TiO 2 S-scheme homojunction was designed and constructed by using a facile surface modification approach whereby oxygen vacancy (OV) and Fe introducing on the TiO 2 nanorod surface. The as-synthesized Fe-TiO 2-x /TiO 2 S-scheme homojunction exhibits positive properties on promoting photocatalytic CO 2 reduction: i) the nanorod structure provides numerous active sites and a radical charge transfer path; ii) the doped Fe and OV not only synergistically enhance light utilization but also promote CO 2 adsorption; iii) the Fe-TiO 2-x /TiO 2 S-scheme homojunction benefits photoexcited charge separation and retains stronger redox capacity. Thanks to those good characters, the Fe-TiO 2-x /TiO 2 homojunction exhibits superior CO 2 reduction performances with optimized CO/CH 4 generation rates of 122/22 μmol g -1 h −1 which exceed those of pure TiO 2 by more than 9.4/7.3 folds and most currently reported catalytic systems. This manuscript develops a facile and universal approach to synthesize well-defined homojunction and may inspire the construction of other more high-efficiency photocatalysts toward CO 2 reduction and beyond.
研究领域:
材料科学
·
环境科学
·
化学工程
·
催化
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yong Xu,Yue Wang,Ping Wang,Yishun Wang,Weili Dai,Jianping Zou,Xubiao Luo
Employing electric energy to convert carbon dioxide (CO 2 ) into valuable small molecules is a potentially practical method in energy storage and greenhouse gas alleviation. A huge challenge for electrocatalytic CO 2 reduction is to reduce overpotential to improve energy efficiency. Herein, we demonstrate that doping alloy Pd 49 Ag 30 Te 4 (PAT) with rare-earth element Tb is beneficial for selective exposure of (1 1 1) crystal plane, which is a highly active crystal plane for producing carbon monoxide (CO). The as-prepared Tb 2.9 PAT exhibited high electrocatalytic performance with 95.7 % CO faradic efficiency at − 0.8 V (vs RHE), far exceeding that of PAT, and coupled with good durability. In situ spectral study and theoretical calculations disclose that the introduction of Tb regulates the d-band center of PAT alloy, weakens the Pd − C bonding ability, and promotes the desorption of *CO in the rate-determining step. This study provides a method for doping induced selective exposure of crystal face, which provides new idea for improving catalytic performance.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
DOI
PubMed
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Qing Lu,Chen Chen,Qian Di,Wanli Liu,Xiaohui Sun,Yongxiao Tuo,Yan Zhou,Yuan Pan,Xiang Feng,Lina Li,De Chen,Jun Zhang
Developing efficient and stable electrocatalysts within a wide potential range is vital for the mature applications of the electrocatalytic CO2 reduction reaction (CO2RR) into value-added chemical products. Herein, we engineered a NC@Ni/C nano-composite featuring a core–shell structure of a pyridinic-N-rich carbon layer encapsulating Ni nanoparticles (NPs) as a highly effective electrocatalyst for CO2RR to CO over a wide potential range. The catalyst demonstrates a high CO Faradaic efficiency (FECO) of >90% in a wide potential range from −0.65 to −1.45 V [vs reversible hydrogen electrode (RHE)] with the maximum FECO of 97% at −1.05 V (vs RHE). Strikingly, it exhibits an excellent stability with a constant current density and a FECO > 95% for 92 h at −1.05 V (vs RHE). Structural studies and DFT calculations further reveal that pyridinic-N doping in the carbon shell of Ni NPs plays a dual role in promoting the CO2RR activity. It not only alleviates the mass transfer limitation of CO2 by enhancing the CO2 adsorption capacity, but it also lowers the reaction energy barrier of the *COOH formation rate-determining step with the electronic structure modulation by Ni. This work may shed more light on the seeking of practical catalysts for high-efficiency electrochemical CO2 reduction over a broad potential window.
研究领域:
材料科学
·
电催化
·
能源转换
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Xi Chen,Qiang Li,Meng Zhang,Juanjuan Li,Songcai Cai,Jing Chen,Hongpeng Jia
CH4 production from CO2 hydrogenation provides a clean approach to convert greenhouse gas CO2 into chemical energy, but high energy consumption in this reaction still restrains its further application. Herein, we use a light-driven CO2 methanation process instead of traditional thermocatalysis by an electrical heating mode, with the aim of greatly decreasing the energy consumption. Under UV–vis–IR light irradiation, the photothermal CO2 methanation over highly dispersed Co nanoparticles supported on Al2O3 (Co/Al2O3) achieves impressive CH4 production rates (as high as 6036 μmol g–1 h–1), good CH4 selectivity (97.7%), and catalytic durability. The high light-harvesting property of the catalyst across the entire solar spectrum coupled with its strong adsorption capacity toward H2, CO2, CO, and abundant active sites are proposed to be responsible for the better photothermocatalytic performance of Co/Al2O3. Furthermore, a novel light-promotion effect is also revealed in CO2 methanation, where UV–vis light irradiation induces oxygen vacancies and improves the proclivity toward adsorption of H2, CO2, and CO, finally resulting in a significant enhancement of the photothermocatalytic activity for CH4 production. By concentrating the low-intensity light (120 mW/cm2) via a Fresnel lens, a photothermal CO2 conversion efficiency of more than 50% with a good CH4 selectivity (76%) is achieved on the optimal catalyst under a dynamic reaction system, which indicates the bright prospect of photothermal CO2 methanation.
研究领域:
化学工程
·
能源科学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Yue Huang,Kai Dai,Jinfeng Zhang,Graham Dawson
Non-stoichiometric W 18 O 49 (WO) prepared by solvothermal method has excellent NIR absorption due to the localized surface plasmon resonance effect caused by oxygen vacancies. This has great potential in the field of using sunlight to convert carbon dioxide into organic fuels. In addition, through the amination of CdSe, the one-dimensional/two-dimensional step-scheme (S-scheme) WO/CdSe-diethylenetriamine (WO/CdSe-D) photocatalyst with electron transmission channels driven by visible light to NIR light is constructed by microwave solvothermal method. The LSPR of WO and the synergistic effect of coupling semiconductors to construct S-scheme heterojunctions can improve light utilization and achieve efficient charge carrier transfer efficiency. The optimized photocatalyst of 35%WO/CdSe-D has the best CO 2 reduction performance compared to WO and CdSe-D, and the yield is 25.37 µmol h –1 g –1 . X-ray photoelectron spectroscopy was used to verify the charge transfer path of the S-scheme WO/CdSe-D heterojunction. This work provides a possibility for the application of non-stoichiometric oxides rich in oxygen vacancies in the field of photocatalytic CO 2 reduction.
研究领域:
材料科学
·
环境科学
·
能源科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Yizheng Tao,Lei Wang,Benxing Li,Jin Huang,Yichang Pan
Interfacial compatibility is a critical prerequisite for maximizing the gas separation pot entail of metal-organic framework (MOF)-based mixed-matrix membranes (MMMs). In this study, an innovative strategy that employs polymers of intrinsic microporosity (PIMs) covalently grafted onto MOF surfaces has been introduced to engineer compatible interfaces through graded interfacial bonding. Through the reaction between PIM-COCl functionalized polymers and ZIF-NH 2 nanoparticles at ambient temperature, amide-bonded PZIF-CONH nanohybrids have been synthesized, which exhibited superior dispersibility in both solvent media and polymer matrices. Notably, the PZIF-CONH nanohybrids retained their intrinsic high porosity without encountering the pore-blocking issues commonly associated with conventional surface modifiers, owing to the microporous nature of PIM materials. The PIM-based surface modification establishes strong interfacial interactions between ZIF-particles and the polyimide matrix, leading to the fabrication of defect-free MMMs. These gas separation membranes have demonstrated significantly enhanced CO 2 permeability and CO 2 /CH 4 selectivity, exceeding the 2008 upper bound. The gas-permeable polymeric modification approach can offer a promising solution for enhancing the stability and separation performance of MMMs.
✓ 已验证
产品关联
DOI
高影响因子
Science Advances
·
2023
·Vol. 9
·期 24
·
IF 13.6
Mingrui Wang,Peng Wang,Guanghui Zhang,Zening Cheng,Mengmeng Zhang,Yulong Liu,Rongtan Li,Jie Zhu,Jianyang Wang,Kai Bian,Yi Liu,Fanshu Ding,Thomas P. Senftle,Xiaowa Nie,Qiang Fu,Chunshan Song,Xinwen Guo
The decomposition of cobalt carbide (Co 2 C) to metallic cobalt in CO 2 hydrogenation results in a notable drop in the selectivity of valued C 2+ products, and the stabilization of Co 2 C remains a grand challenge. Here, we report an in situ synthesized K-Co 2 C catalyst, and the selectivity of C 2+ hydrocarbons in CO 2 hydrogenation achieves 67.3% at 300°C, 3.0 MPa. Experimental and theoretical results elucidate that CoO transforms to Co 2 C in the reaction, while the stabilization of Co 2 C is dependent on the reaction atmosphere and the K promoter. During the carburization, the K promoter and H 2 O jointly assist in the formation of surface C * species via the carboxylate intermediate, while the adsorption of C * on CoO is enhanced by the K promoter. The lifetime of the K-Co 2 C is further prolonged from 35 hours to over 200 hours by co-feeding H 2 O. This work provides a fundamental understanding toward the role of H 2 O in Co 2 C chemistry, as well as the potential of extending its application in other reactions.
研究领域:
催化化学
·
化学工程
·
材料科学
·
可持续能源
·
多相催化
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）