APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jiaqi Qiu,Mingnv Guo,Zhongqing Yang,Ziqi Wang,Ruiming Fang,Jiang He,Jingyu Ran
A series of novel iodine substitution and oxygen vacancy double defects Bi 2 MoO 6 nanosheets for enhanced photocatalytic reduction of CO 2 is reported, which exhibited superior CO 2 photocatalytic activity and CH 4 selectivity under full solar spectrum illumination. Bi 2 MoO 6 -I2 (the molar ratio of I to Mo is 0.13) has the highest photocatalytic activity, its CO yield is 2.0 times that of pure Bi 2 MoO 6 , the CH 4 yield is 12.2 times that of pure Bi 2 MoO 6 , and the CH 4 selectivity reaches 5.3 times that of pure Bi 2 MoO 6 . Its structure and physicochemical properties were investigated by material characterizations, photoelectrochemical tests and DFT calculations. The enhancement in CO 2 conversion and CH 4 selectivity benefit from: (1) Larger specific surface areas and smaller nanosheets thicknesses facilitate carrier migration; (2) More suitable band structure promotes the reduction of CO 2 ; (3) Insertion of impurity energy levels in the band gap enables efficient jumping of photogenerated electrons; (4) Double defects contribute to efficient CO 2 adsorption and activation; (5) Promoting highly selective conversion of CO 2 to CH 4 by optimising the formation energy of reaction intermediates.
研究领域:
材料科学
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环境科学
·
光催化
✓ 已验证
DOI
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
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材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2019
·
IF 4.888
Lei Zhang,Hao Wang,Chengguang Yang,Xiaopeng Li,Jian Sun,Hui Wang,Peng Gao,Yuhan Sun
The present work reports on the promoting effects of rare earth elements (La, Ce and Y) to FeK/Al 2 O 3 catalysts on liquid hydrocarbons from CO 2 hydrogenation. The addition of La, Ce and Y can both improve the selectivity of C 5+ hydrocarbons and reduce the selectivity of CH 4 . The C 5+ selectivity can enhance to about 60 % with CH 4 selectivity of around 11 % at CO 2 conversions above 20 %. N 2 adsorption–desorption, in situ XRD, H 2 –TPR, CO 2 /H 2 –TPD, HRTEM and XPS are used to characterize the FeK/Al 2 O 3 and FeK/M-Al 2 O 3 (M = La, Ce, Y) catalysts. The results show that the introduction of rare earth elements into the FeK/Al 2 O 3 catalyst obviously reduces the adsorption of H 2 , which suppresses the CH 4 formation. On the other hand, rare earth elements also promote the adsorbed CO 2 species, which leads to the enhanced liquid hydrocarbons selectivity. Finally, the tailored CO 2 /H 2 ratio of CO 2 and H 2 adsorption on the catalyst surface can influence the catalyst activity and the product selectivity evidently.
研究领域:
催化化学
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材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·Vol. 30
·期 68
·e202402516
·
IF 3.9
Chaoyang Yang,Junlei Zhang,Weiping Liu,Yao Cheng,Xueyi Yang,Wanglei Wang
Graphical This study investigated the impact of H 2 /CO 2 partial pressure ratios on CO 2 methanation using Ni/CeO 2 . Results show elevated H 2 /CO 2 ratios enhance CO 2 conversion and CH 4 selectivity, achieving complete methanation at 250 °C and 100 % selectivity at 400 °C. In-situ DRIFTS analysis indicates formate pathway dominance at higher ratios, key for CH 4 production and CO 2 mitigation strategies. On the way to carbon neutrality, directly catalyzing atmospheric CO 2 into high-value chemicals might be an effective approach to mitigate the negative impacts of rising airborne CO 2 concentrations. Here, we pioneer the investigation of the influence of the H 2 /CO 2 partial pressure ratio (PPR) on air-level CO 2 methanation. Using Ni/CeO 2 as a case catalyst, increasing H 2 /CO 2 PPR significantly improves low-temperature CO 2 conversion and high-temperature CH 4 selectivity, i. e., from 10 of H 2 /CO 2 PPR on, CO 2 is completely methanized at 250 °C, and nearly 100 % CH 4 selectivity is achieved at 400 °C. 100-hour stability tests demonstrate the practical application potential of Ni/CeO 2 at 250 °C and 400 °C. In-situ DRIFTS reveal that reinforced formate pathway by increasing H 2 /CO 2 PPR is responsible for the high CH 4 yield. In contrast, even though the CO pathway dominated CO 2 conversion on Ni is enhanced by rising H 2 /CO 2 PPR, but at a high reaction temperature, the promoted CO desorption still leads to lower CH 4 selectivity. This work offers deep insights into the direct air-level CO 2 resourceization, contributing to the achievement of airborne CO 2 reductions.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 14
·6720-6728
·
IF 3.925
Jie Shen,Qi Sun,Jun Cao,Peng Wang,Weilin Jia,Suyang Wang,Ping Zhao,Zepeng Wang
Zeolite LTA, with high porosity and uniform pore distribution, has been widely used in the gas adsorption field. In this paper, a 1.38 nm thick two-dimensional zeolite LTA was synthesized from kaolin, changing the cubic morphology of the traditional zeolite LTA. SEM and TEM images showed that the zeolite LTA exhibited a lamellar structure. In a comparative experiment with CO2 adsorption at different temperatures, the 2D zeolite LTA with a large specific surface area could capture more CO2 than the conventional 3D zeolite LTA. In addition, the CO2/CH4 selectivity of the 2D Zeolite LTA was 76.78 at 298 K.
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
Advanced Science
·
2024
·Vol. 11
·期 30
·2401990
·
IF 14.3
Qinhui Guan,Weiguang Ran,Dapeng Zhang,Wenjuan Li,Na Li,Baibiao Huang,Tingjiang Yan
Photocatalytic CO 2 reduction is considered as a promising strategy for CO 2 utilization and producing renewable energy, however, it remains challenge in the improvement of photocatalytic performance for wide-band-gap photocatalyst with controllable product selectivity. Herein, the sulfur-doped In(OH) 3 (In(OH) x S y -z) nanocubes are developed for selective photocatalytic reduction of CO 2 to CH 4 under simulated light irradiation. The CH 4 yield of the optimal In(OH) x S y -1.0 can be enhanced up to 39 times and the CH 4 selectivity can be regulated as high as 80.75% compared to that of pristine In(OH) 3 . The substitution of sulfur atoms for hydroxyl groups in In(OH) 3 enhances the visible light absorption capability, and further improves the hydrophilicity behavior, which promotes the H 2 O dissociation into protons (H * ) and accelerates the dynamic proton-feeding CO 2 hydrogenation. In situ DRIFTs and DFT calculation confirm that the non-metal sulfur sites significantly weaken the over-potential of the H 2 O oxidation and prevent the formation of ·OH radicals, enabling the stabilization of * CHO intermediates and thus facilitating CH 4 production. This work highlights the promotion effect of the non-metal doping engineering on wide-band-gap photocatalysts for tailoring the product selectivity in photocatalytic CO 2 reduction.
研究领域:
材料科学
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环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaoyan Zhang,Wenkang Ni,Xuanyu Yue,Zhijie Wang,Zizhong Zhang,Ke Wang,Wenxin Dai,Xianzhi Fu
Converting CO 2 into CO, CH 4 , and other hydrocarbons using solar energy presents a viable approach for addressing energy shortages. In this study, photocatalysts with S-deficient WO 3 /Zn 3 In 2 S 6 (WO 3 /V S -ZIS) S-scheme heterojunctions have been successfully synthesized. Under UV–vis light irradiation, 20 %WO 3 /V S -ZIS demonstrated significantly improved CO 2 reduction activity and CH 4 selectivity. Detailed characterization and density functional theory (DFT) calculations reveal that the enhanced performance is due to the synergistic optimization of the S-scheme heterojunction and sulfur vacancies (V S ) for CO 2 reduction. The presence of V S aids in the adsorption and activation of CO 2 and enhances the separation of charge carriers. The 2D/2D S-scheme heterostructure assembled with WO 3 nanosheets not only accelerates the migration and separation of photoexcited charge carriers but also improves the adsorption of H 2 O and the formation of V S , thereby increasing the adsorption and activation of CO 2 and facilitating the protonation of CO* to produce CH 4 . This study clarifies the synergistic effect of V S and S-scheme heterostructures in improving photocatalytic performance, offering valuable insights into the photoactivation process of CO 2 at V S in S-scheme heterojunctions.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Jing Yang,Shiying Fan,Xinyong Li,Jing Wang,Yiyuan Tao,Jingang Wang,Moses O. Tade,Shaomin Liu
Electrochemical dechlorination of dichloromethane (DCM) to high-value methane not only reduces carbon emission and environmental pollution but also alleviates energy shortages. In this study, a series of carbon-confined NiCo2O4−β/Cx (NCO4−β/Cx, x = 0, 0.5, 1, 2, 3) with hierarchical nano-microflower structures were successfully constructed via combining the hydrothermal method and dopamine in situ polymerization, which were utilized as electrocatalysts for electrochemical dechlorination of DCM. The as-prepared NCO4−β/C1 showed remarkable electrocatalytic dechlorination performance of DCM with a high methane selectivity of 87% and methane Faradaic efficiency of 17%, where the production rate of methane is up to 3538.25 μmol g–1 h–1 at −2.98 V (vs Ag/AgCl/Me4NCl). Notably, it could be experimentally proved that nickel cobaltite encapsulated in the carbon layer may accelerate the charge transfer and then build up the dechlorination activity. Additionally, two possible dichlorination mechanisms of DCM to methane are theoretically confirmed at the Ni active sites, which is proved by DFT calculations. This study presents promising ideas for developing efficacious dechlorination electrocatalysts and the efficient transformation of chlorinated volatile compounds (Cl-VOCs) to value-added methane in an environmentally benign manner.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 45
·2302022
·
IF 13.3
Hai-Bing Zhao,Jia-Nan Huang,Qi Qin,Hong-Yan Chen,Dai-Bin Kuang
Rational design and facile synthesis of efficient environmentally friendly all-inorganic lead-free halide perovskite catalysts are of great significance in photocatalytic CO 2 reduction. Aiming at photogenerated charge carrier separation and CO 2 reaction dynamics, in this paper, a CsCuCl 3 /Cu nanocrystals (NCs) heterojunction catalyst is designed and synthesized via a simple acid-etching solution process by using Cu 2 O as the sacrificed template. Due to the disproportionation reaction of Cu 2 O induced by concentrated hydrochloric acid, Cu NCs can be deposited onto the surface of CsCuCl 3 microcrystals directly and tightly. As revealed by photoelectrochemical analysis, in situ Fourier transform infrared spectra, etc., the Cu NCs contribute a lot to extracting photoelectrons of CsCuCl 3 to improve the charge separation efficiency, regulating the CO 2 adsorption and activation, and also stabilizing the reaction intermediates. Therefore, CsCuCl 3 /Cu heterojunction exhibits a total electron consumption rate of 58.77 µmol g −1 h −1 , which is 2.9-fold of that of single CsCuCl 3 . Moreover, high CH 4 selectivity of up to 92.7% is achieved, which is much higher than that of CsCuCl 3 (50.4%) and most lead-free halide perovskite-based catalysts. This work provides an ingenious but simple strategy to rationally design cocatalysts in situ decorated perovskite catalysts for manipulating both the catalytic activity and the product selectivity.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2020
·
IF 3.871
Chumei Ye,Xingyu Wu,Hong Wu,Leixin Yang,Yanxiong Ren,Yingzhen Wu,Yutao Liu,Zheyuan Guo,Rui Zhao,Zhongyi Jiang
Membrane-based separations are of energy-efficient and environmentally benign attributes for biogas energy developments. Membranes from polymers of intrinsic microporosity (PIMs) often suffer from low selectivity. In this study, remarkable enhancements in CO 2 /CH 4 selectivity of PIM-1 membranes are achieved by incorporating nano-sized ZIF-67 (ZIF-S) filler with a larger specific surface area and a better compatibility, thereby fortifying the interactions with PIM-1 matrix and effectively alleviating nonselective interfacial voids. For the resulting PIM-1/ZIF-S membranes, a maximum CO 2 /CH 4 selectivity of 21.1 was acquired with 15 wt% loading of ZIF-S, an increase of 69.40% compared with the pristine PIM-1 membrane, along with an associated CO 2 permeability above 2800 Barrer. To elucidate gas transport behaviors within membranes, a modified Maxwell model is developed and the calculation results match well with the experimental data. The strategy of incorporating framework nanofillers into membranes may find promising applications in enhancing the selectivity of highly permeable polymer membranes.
研究领域:
材料科学
·
环境工程
·
能源技术
✓ 已验证
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2019
·Vol. 33
·期 11
·e5208
·
IF 3.259
Baowei Wang,Chengyu Wang,Wenxian Yu
Mo 2 C/Al 2 O 3 catalyst was prepared by the impregnation method with urotropine and ammonium paramolybdate. The catalytic effect of Mo 2 C as a typical transition-metal carbide in sulfur-resistant methanation was studied. The catalysts prepared were characterized by N 2 adsorption–desorption, X-ray diffraction, transmission electron microscopy, H 2 -temperature-programmed reduction, and Raman spectra, with the results confirming the formation of β-molybdenum carbide on the surface of the catalysts. Studies on catalysts with different loading doses indicate that the optimal loading of Mo 2 C/Al 2 O 3 is about 15 wt.%, which enables CO conversion rate of up to 47%, with methane selectivity of up to 53%. This work further explored the effect of different concentrations of H 2 S in the raw gas on the performance of the catalyst, with the results showing that high concentration of H 2 S (>1500 ppm) can lead to sulfuration of active species on the catalyst, while resulting in a decrease in the catalytic activity.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Chenxi Wang,Gang Lv,Yunqiang Li,Ye Liu,Chonglin Song
The selective catalytic reduction of nitrogen oxides by methane (CH 4 /NO X -SCR) is a potential technique for the abatement of the NO X emissions from lean-burn GDI engines, due to the excellent thermal stability of CH 4 . This work focuses on the promotion of In/SSZ-13 catalysts by Ce modification for the CH 4 /NO X -SCR performance at high temperatures. A series of In/SSZ-13 and Ce-In/SSZ-13 catalysts were prepared using the wetness impregnation method. The effects of Ce modification on the catalytic performance were analysed in detail using the scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, ultraviolet-visible diffuse reflectance spectrum and temperature-programmed desorption/reduction techniques. The results show that the Ce modification significantly enhances the high-temperature activity of the In/SSZ-13 catalysts for the NO X -SCR reaction, especially for the 5 wt% Ce-15 wt% In/SSZ-13 sample which has more than 75% NO X conversion at 390–700 °C. In addition, the Ce modification enhances the water vapor tolerance of the catalyst sample. The Ce modification increases not only the concentration of surface chemisorption oxygen species, but also the relative amount of InO + species which serve as the main active sites for CH 4 activation. Furthermore, the incorporation of Ce into In/SSZ-13 greatly promotes NO X adsorption on the catalyst surface. Most importantly, the Ce modification makes In species well-dispersed on the catalyst surface and thus suppresses the formation of bulk In 2 O 3 species which are more active for the CH 4 non-selective oxidation. The combination of all these effects results in the Ce-In/SSZ-13 samples with the superior catalytic activity .
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
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