Advanced Science
·
2022
·Vol. 9
·期 16
·2105292
·
IF 17.521
Yawen Jiang,Xinyu Wang,Delong Duan,Chaohua He,Jun Ma,Wenqing Zhang,Hengjie Liu,Ran Long,Zibiao Li,Tingting Kong,Xian Jun Loh,Li Song,Enyi Ye,Yujie Xiong
Structural reconstruction is a process commonly observed for Cu-based catalysts in electrochemical CO 2 reduction. The Cu-based precatalysts with structural complexity often undergo sophisticated structural reconstruction processes, which may offer opportunities for enhancing the electrosynthesis of multicarbon products (C 2+ products) but remain largely uncertain due to various new structural features possibly arising during the processes. In this work, the Cu 2 O superparticles with an assembly structure are demonstrated to undergo complicated structure evolution under electrochemical reduction condition, enabling highly selective CO 2 -to-C 2+ products conversion in electrocatalysis. As revealed by electron microscopic characterization together with in situ X-ray absorption spectroscopy and Raman spectroscopy, the building blocks inside the superparticle fuse to generate numerous grain boundaries while those in the outer shell detach to form nanogap structures that can efficiently confine OH − to induce high local pH. Such a combination of unique structural features with local reaction environment offers two important factors for facilitating C−C coupling. Consequently, the Cu 2 O superparticle-derived catalyst achieves high faradaic efficiencies of 53.2% for C 2 H 4 and 74.2% for C 2+ products, surpassing the performance of geometrically simpler Cu 2 O cube-derived catalyst and most reported Cu electrocatalysts under comparable conditions. This work provides insights for rationally designing highly selective CO 2 reduction electrocatalysts by controlling structural reconstruction.
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
DOI
高影响因子
Reaction Chemistry & Engineering
·
2024
·Vol. 10
·期 1
·203-213
·
IF 3.4
Ning Ma,Liu Yang,Zhenchang Fang,Kaijia Jiang,Xinling Li,Zhen Huang
Deficiencies such as high viscosity, volatility, and rich phase precipitation limited the engineering application of non-aqueous absorbents. A series of high boiling point solvent screening experiments were conducted to develop an absorption saturated solution with a homogeneous phase at low viscosity (14.71 mPa s) in this study. Further addition of polyamines increased the absorption capacity by 42% (3.55 mol CO2 per kg). The 13C NMR results indicated that in the DETA/MEA/NMF blended amine system, MEA was involved in the deprotonation process of DETA zwitterions as proton acceptors. Quantum chemical calculations were utilized to compare the energies of each possible single-step reaction, providing insights into the reaction pathways of the blended amine system. The rate constant of the MEA/CO2 reaction was found to be 1.98 times that of the DETA/CO2 reaction, indicating lower reaction activity, consistent with NMR results. In addition, the results of the analysis of weak interactions revealed that the hydrogen bonds were key factors affecting the viscosity change and precipitation in non-aqueous absorbents, providing a new method for designing novel low-viscosity non-aqueous absorbents. The combination of theoretical analysis and experimental results underscores the potential of the blended amine non-aqueous absorbent as a feasible alternative for the industrial applications of CO2 capture.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2024
·
IF 7.2
Luqman Abdullahi Sani,Haolong Bai,Zifu Xu,Liangliang Fu,Yining Sun,Xiaorui Huang,He Gao,Xuejing Liu,Dingrong Bai,Zhanguo Zhang,Fabing Su,Jiao Liu,Guangwen Xu
Ni/Al 2 O 3 catalysts (noted as Ni/Al-350, Ni/Al-500, and Ni/Al-700, respectively) were synthesized by a facile solution combustion method but at different combustion temperatures (350 °C, 500 °C, and 700 °C, respectively). For comparison, Ni/Al 2 O 3 (noted as Ni/Al-100) was also prepared by the impregnation method and applied in the methanation reaction. The Ni/Al 2 O 3 synthesized at the combustion temperature of 350 °C showed better performance than the others at higher combustion temperatures, and the activity for CO 2 methanation followed an order of Ni/Al-350 > Ni/Al-500 > Ni/Al-700 > Ni/Al-100. The increase in the combustion temperature decreased active sites for the H 2 and CO 2 adsorption, which could be associated with the reduced Ni dispersion and basic sites, thus lowering its activity and increasing its carbon deposition rate.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2016
·Vol. 32
·期 3
·605-610
·
IF 0.844
CHEN Feng-Feng,DONG Yan,SANG Xiao-Yan,ZHOU Yan,TAO Duan-Jian
Four tetrabutylphosphonium carboxylate ionic liquids ([P4444][CA]) were prepared, and their densities, viscosities, refractive indices, and conductivities were measured and correlated with thermodynamic and empirical equations in the temperature range of 298.15-348.15 K.
The influence of temperature on these four properties of [P4444][CA] was discussed, and their thermal expansion coefficient values were calculated. The CO2 absorption capacity of [P4444][CA] was studied at 313.15 K and 100 kPa. The results indicated that [P4444][Buty]
had the highest CO2 capture capacity among these ionic liquids, with an absorption capacity of 0.4 mol·mol-1 and balance time of less than 5 min.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
Advanced Energy Materials
·
2019
·Vol. 9
·期 18
·1900364
·
IF 24.884
Chenyan Guo,Peng He,Rongrong Cui,Qi Shen,Nianjun Yang,Guohua Zhao
Electrochemical CO 2 reduction (ECCO 2 R) requires electrons, for example, from oxygen evolution reaction (OER). However, such a multiple-electron-involved reaction is complicated and kinetically slow, leading to high overpotential. Herein, OER is replaced with photoelectrocatalytic phenol oxidation reaction (PECPOR) that provides electrons for ECCO 2 R. In an integrated cell, ECCO 2 R is conducted on the cathode of Cu nanowires and PECPOR is performed on the anode of SnO 2 and Sb coated TiO 2 nanotubes. Significant improvement of ECCO 2 R into CO and hydrocarbons is realized when PECPOR is conducted at a high current density. The use of this integrated system results in the reduction of the specific energy consumption by a factor of 51.33%, compared with the utilization of two half-cells for individual ECCO 2 R and PECPOR. This study thus proposes a novel strategy to couple ECCO 2 R with PECPOR and eventually to tackle the problems of environmental pollution and energy crisis.
研究领域:
环境科学
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电化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Di Li,Qin Li,Yimeng Zhou,Qiong Zhang,Qianjin Ye,Ran Yang,Deli Jiang
Steering selectivity in photocatalytic conversion of CO2, especially toward deep reduction products, is vital to energy and environmental goals yet remains a great challenge. In this work, we demonstrate a facet-dependent photocatalytic selective reduction of CO2 to CH4 in Cu-doped TiO2 catalysts exposed with different facets synthesized by a topological transformation from MIL-125 (Ti) precursors. The optimized round cake-like Cu/TiO2 photocatalyst mainly exposed with the (001) facet exhibited a high photocatalytic CO2 reduction performance with a CH4 yield of 40.36 μmol g–1 h–1 with a selectivity of 94.1%, which are significantly higher than those of TiO2 (001) (4.70 μmol g–1 h–1 and 52.6%, respectively), Cu/TiO2 (001 + 101) (18.95 μmol g–1 h–1 and 69.6%, respectively), and Cu/TiO2 (101) (14.73 μmol g–1 h–1 and 78.9%, respectively). The results of experimental and theoretical calculations demonstrate that the Cu doping dominating the promoted separation and migration efficiencies of photogenerated charges and the preferential adsorption on (001) facets synergistically contribute to the selective reduction of CO2 to CH4. This work highlights the significance of synergy between facet engineering and ion doping in the design of high-performance photocatalysts with respect to selective reduction of CO2 to multielectron products.
研究领域:
材料科学
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环境科学
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能源科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 11
·1-17
·
IF 2.8
Pan Deng,Wang Yanan,Lin Liwei,Zhang Yuzhe,Zhou Man,Li Zhongyu,Xu Song
Photothermal catalytic CO 2 reduction can combine photocatalysis and thermal catalysis by using full-spectrum solar energy to convert CO 2 into high value-added chemicals. This can effectively alleviate the problems of excessive CO 2 emissions and thermal catalytic energy waste. In this paper, a novel catalyst was prepared using Ce-MOF as a precursor to generate Cu/Ni/CeO 2 for efficient reduction of CO 2 to CO by hydrogenation. Due to the rod-like structure of CeO 2 and the high dispersion of Cu and Ni nanoparticles, 10%Cu 5%Ni CeO 2 can achieve a catalytic activity of 54.21 mmol g −1 h −1 in the full solar spectrum. The supported Cu and Ni metals are the active sites for catalytic reduction. Meanwhile, Cu and Ni enhanced the light absorption ability of the catalyst and the surface temperature under illumination. This is due to the hot charge carriers generated by LSPR effect in Ni and Cu metal nanoparticles, which can dissipate energy through local heating, thus increasing the temperature of the catalyst under illumination. It can be found that the CO 2 reduction activity of photo-assisted thermocatalysis is higher than that of thermal catalysis under the same conditions. Therefore, the combined effect of the electrons generated by UV–Vis light and the heating effect of near-infrared light on catalyst could improve the catalytic activity. This work might provide a potential strategy for efficient photothermal reduction of CO 2 in the future.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
VACUUM
·
2024
·
IF 3.8
Kaiting Yang,Xiongtao Lv,Jingwen Meng,Huiqing Wang,Lin Guo,Xin Li,Fengyun Su,Qing Lan,Zhengdao Li,Wei Wang,Yuwei Guo,Xiaoli Jin,Haiquan Xie
Photothermal catalytic reduction of CO 2 into high value-added C 2 hydrocarbon products is a promising method for efficient CO 2 conversion. However, current photocatalysts still encounter obstacles including limited photoabsorption range, rapid recombination of photogenerated carriers , and inadequate surface active sites. Herein, Bi 4 O 5 Br 2 co-modified with oxygen vacancy (OV) and metal bismuth (Bi) (Bi 4 O 5 Br 2 -OV@Bi) has been prepared to optimize these crucial issues. Bi 4 O 5 Br 2 -OV@Bi delivers a remarkably improvement in CO 2 photothermal conversion, reflecting by the notable increase in C 1 (CO and CH 4 ) and newly generated C 2 (C 2 H 4 and C 2 H 6 ) products compared to pristine Bi 4 O 5 Br 2 . In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) spectrometry reveals that OC−COH* intermediate promotes the C–C coupling for produce C 2 hydrocarbons. This study strengthens the understanding of metal modification and defect engineering for forming C 2 hydrocarbons on bismuth-based photocatalysts .
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Xianying Wang,Yingshu Wang,Meichao Gao,Jinni Shen,Xipeng Pu,Zizhong Zhang,Huaxiang Lin,Xuxu Wang
Construction of composite semiconductors is an effective solution to elevate the efficiency of photocatalysis by prolonging lifetime of photogenerated hole and electrons. Herein, a heterojunction structure composite BiVO 4 /Bi 4 Ti 3 O 12 was synthesized via a facile in situ hydrothermal condition. The novel composite photocatalyst has excellent photocatalytic ability to reduce CO 2 with H 2 O into CH 3 OH and CO. The BiVO 4 /10 % Bi 4 Ti 3 O 12 sample shows the highest yields of CH 3 OH and CO up to 16.6 and 13.29 μmol g −1 h −1 , which was 12.39 and 5.68 times higher than that of pure BiVO 4 , and 9.88 and 2.80 times higher than that of pure Bi 4 Ti 3 O 12 , respectively. Such a high activity is attributed to the type II heterojunction structure which significantly enhances separation of photogenerated carriers and promotes collaboration between the water oxidation on the Bi 4 Ti 3 O 12 and the CO 2 reduction on BiVO 4 . The photocatalytic reaction mechanism of CO 2 on the composite was proposed according to experiment results.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Shuangqi Song,Hong Li,Jingde Li,Yanqin Yang
Mixed-matrix membranes (MMMs), developed through the combination of solid fillers with polymer matrices, represent an effective approach addressing the persistent challenge of balancing permeability and selectivity in polymer membrane. Diethylenetriamine-functionalized porous material of PP-DETA, which is synthesized from porous organic polymer of PP via one-step diethylenetriamine grafting, is an ideal material for MMMs production. However, designing and optimizing PP-DETA for high-performance CO 2 separation membranes remains a challenge. Herein, we develop an improved PP-DETA material, designated as PP-DETA-cPIM-1, by covalently attaching a carboxylated polymer of intrinsic microporosity (cPIM-1) network layer onto the PP-DETA surface. Membranes prepared from this PP-DETA-cPIM-1 filler and PIM-1 matrix demonstrate enhanced interfacial adhesion and stronger mechanical properties in comparison to the counterparts with the same loading of PP-DETA. The incorporation of PP-DETA-cPIM-1 into MMMs establishes an enhanced filler/polymer interface that facilitates the selective transport of CO 2 through the filler, while simultaneously improving membrane stability and suppressing physical aging. Specifically, with 5 wt% loading of PP-DETA-cPIM-1 filler, the MMM is able to enhance the CO 2 /N 2 selectivity and CO 2 permeability by 52.3 % and 25.3 %, respectively, exceeding the upper bound established in 2008. Furthermore, PP-DETA-cPIM-1/PIM-1 MMMs display superior anti-aging ability for 180 days of aging.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Guiming Xie,Xingyang Bai,Yanrui Niu,Runduo Zhang,Jian Liu,Qingyuan Yang,Zhou-Jun Wang
Making use of novel materials to develop efficient catalysts is one of the research hotspots for CO2 hydrogenation to methanol. Herein, UiO-66, a typical Zr-MOF, was modified by ethylene diamine tetraacetic acid (EDTA) to serve as a substrate for the synthesis of AuCu bimetallic catalysts. The resultant AuCu@UiO-66-EDTA catalyst exhibited a superior methanol production rate, which delivered a high space-time yield of methanol (3.34 gMeOH gmetal–1 h–1) at 250 °C and 3.0 MPa. The EDTA modification was found to effectively confine AuCu nanoparticles inside the framework of MOFs, which significantly reduced the metal particle size and enriched the oxygen vacancy concentration. As a consequence, more active sites were generated for methanol synthesis. Moreover, the AuCu@UiO-66-EDTA catalyst yielded more favorable reaction intermediates that could be converted to methanol at a faster rate. This work develops unique MOFs-encapsulated bimetallic catalysts and illuminates the positive effect of confinement.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
Nanoscale
·
2025
·
IF 5.1
Yubin Zheng,Zhe Lu,Zhisheng Shi,Lu Wang,Shuyuan Yang,Runzhi Cao,Gao Wa,Xin Zhou,Yong Yang,Chong Sheng,Yong Zhou,Zhigang Zou
A highly dispersed NiCo alloy catalyst derived from NiCo bimetallic–organic framework nanosheets was synthesized for efficient photothermal catalysis for CO2 hydrogenation to methane. The NiCo bimetal catalyst achieves a CH4 production rate of 55.60 mmol g−1 h−1 with only a 18.82% decline in performance after 86 hours under atmospheric pressure at selected 290 °C and continuous flow reaction. In situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) reveals the synergistic and complementary roles of light and heat in photothermal catalysis. The thermochemical process drives the reverse water–gas shift reaction to form a *CO intermediate, a key intermediate for the formation of CH4, and light irradiation-generating strong near field from the surface plasma resonance of NiCo bimetals promotes the subsequent *CO hydrogenation step to form *CHO, the rate-determining step for the hydrogenation of CO2 into CH4. Meanwhile, density functional theory (DFT) calculations suggest that the NiCo bimetallic catalyst can also lower the energy barrier of *CO hydrogenation, facilitating the formation of *CHO.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）