Materials
·
2023
·Vol. 16
·期 20
·6665
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IF 3.4
Manying Sun,Chuanwei Zhu,Su Wei,Liuyun Chen,Hongbing Ji,Tongming Su,Zuzeng Qin
Photocatalytic CO2reduction is a tactic for solving the environmental pollution caused by greenhouse gases. Herein, NH4H2PO4was added as a phosphorus source in the process of the hydrothermal treatment of melamine for the first time, and phosphorus-doped hollow tubular g-C3N4(x-P-HCN) was fabricated and used for photocatalytic CO2reduction. Here, 1.0-P-HCN exhibited the largest CO production rate of 9.00 μmol·g−1·h−1, which was 10.22 times higher than that of bulk g-C3N4. After doping with phosphorus, the light absorption range, the CO2adsorption capacity, and the specific surface area of the 1.0-P-HCN sample were greatly improved. In addition, the separation of photogenerated electron–hole pairs was enhanced. Furthermore, the phosphorus-doped g-C3N4effectively activated the CO2adsorbed on the surface of phosphorus-doped g-C3N4photocatalysts, which greatly enhanced the CO production rate of photocatalytic CO2reduction over that of g-C3N4.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 10
·3422-3427
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IF 6.119
Yuqing Shao,Xinkui Wang,Zhaolin Dou,Xiaoyu Liang,Xinxin Zhang,Min Pang,Qiang Xu,Min Ji,Min Wang
Solar-driven CO2 conversion into fuels and sustainable energy has attracted increasing attention around the world. However, the efficiency of the transformation remains relatively low due to the rapid recombination of photogenerated charge carriers. In this work, we prepared a ZnIn2S4–ZnAlOx nanocomposite for visible light driven CO2 reduction. The thin layered structure facilitated the photoinduced charge carrier separation and transfer, and also gave excellent adsorption ability towards CO2 molecules. Such a nanocatalyst exhibited excellent activity in visible-light driven CO2 reduction with a CO optimal formation rate of 1100 μmol g−1 h−1, which is 5 times that over bulk ZnIn2S4, and the CO/H2 ratio was increased from 0.2 over bulk ZnIn2S4 to 1.5 over the ZnIn2S4–ZnAlOx composite. In situ FT-IR experiments indicated that CO2 was reduced on ZnIn2S4–ZnAlOx following a COOH* pathway. This work gives insights into the mechanism of the photocatalytic CO2 reduction reaction and inspiration to construct novel heterostructure materials for application in energy and environmental catalysis.
研究领域:
材料科学
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环境催化
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光化学
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能源转化
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Sisi Lin,Xinkui Wang,Xiaoyu Liang,Xinxin Zhang,Min Wang
Photocatalytic reduction of CO2 to high value-added chemicals and fuels has received widespread attention. However, the higher thermodynamic stability of CO2 greatly limits its conversion efficiency. Frustrated Lewis pairs (FLPs) have been well-established to be very effective in CO2 activation. In this work, we prepared ZnIn2S4–AlOOH (ZIS–AlOOH) composites for visible-light-driven CO2 reduction. The Lewis basic OHv sites on the AlOOH surface (one H removed from OH) and an adjacent Lewis acidic unsaturated Al site (Al3+unsatur.) form the FLPs. The composite structure facilitated light absorption, CO2 adsorption activation, and separation of photogenerated carriers, thus improving the CO2 photoreduction activity (CO generation rate of 510.3 μmol g−1 h−1), and suppressing hydrogen evolution with the CO/H2 ratio increasing from 0.38 for ZnIn2S4 (ZIS) to 0.84 for ZIS–AlOOH. This work elucidates a rational strategy for the construction of efficient photocatalysts and provides insight into the mechanism of the photocatalytic CO2 reduction reaction.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
·
IF 17.694
Shangguan Wenchao,Liu Qing,Wang Ying,Sun Ning,Liu Yu,Zhao Rui,Li Yingxuan,Wang Chuanyi,Zhao Jincai
Achieving CO 2 reduction with H 2 O on metal photocatalysts and understanding the corresponding mechanisms at the molecular level are challenging. Herein, we report that quantum-sized Au nanoparticles can photocatalytically reduce CO 2 to CO with the help of H 2 O by electron-hole pairs mainly originating from interband transitions. Notably, the Au photocatalyst shows a CO production rate of 4.73 mmol g −1 h −1 (~100% selectivity), ~2.5 times the rate during CO 2 reduction with H 2 under the same experimental conditions, under low-intensity irradiation at 420 nm. Theoretical and experimental studies reveal that the increased activity is induced by surface Au–O species formed from H 2 O decomposition, which synchronously optimizes the rate-determining steps in the CO 2 reduction and H 2 O oxidation reactions, lowers the energy barriers for the *CO desorption and *OOH formation, and facilitates CO and O 2 production. Our findings provide an in-depth mechanistic understanding for designing active metal photocatalysts for efficient CO 2 reduction with H 2 O.
研究领域:
化学
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材料科学
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环境科学
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催化
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Feng Yue,Mengke Shi,Cong Li,Yang Meng,Shuo Zhang,Lan Wang,Yali Song,Jun Li,Hongzhong Zhang
Directly capturing CO 2 in ambient air and converting it into value-added fuels using photocatalysis is a potentially valuable technology. In this study, Cu-porphyrin (tetrakis-carboxyphenyl porphyrin copper, CuTCPP) was innovatively anchored on the surface of TiO 2 (titanium dioxide) nanosheets to form an S-scheme heterojunction. Based on this, a photocatalytic reaction system for stably converting CO 2 in ambient air into value-added fuels at the gas–solid interface was constructed without addition of sacrificial agents and alkaline liquids. Under the illumination of visible light and sunlight, the evolution rate of CO is 56 μmol·g −1 ·h −1 and 73 μmol·g −1 ·h −1 , respectively, with a potential CO 2 conversion rate of 35.8 % and 50.4 %. The enhanced of photocatalytic performance is attributed to the introduction of CuTCPP, which provides additional active sites, significantly improves capture capacity of CO 2 and the utilization of electrons. Additionally, the formation of S-scheme heterojunction expands the redox range and improves the separation efficiency of photo-generated charges.
研究领域:
光催化
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材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 12
·期 2
·606-612
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IF 6.119
Yuqing Shao,Zhaolin Dou,Xiaoyu Liang,Xinxin Zhang,Min Ji,Min Pang,Min Wang,Xinkui Wang
The photocatalytic reduction of CO2 into valuable fuels and sustainable energy has a promising future, yet remains a challenge due to low charge separation efficiency and inadequate active sites. We find that ZnIn2S4-loaded secondary amine-functionalized organic silica (ZnIn2S4/NH–SiO2) was effective for visible-light driven CO2 photocatalytic reduction. The ZnIn2S4/NH–SiO2 with 40% ZnIn2S4 content achieves a CO production rate of 1304.8 μmol g−1 h−1 at room temperature, which is about 3 times higher than that of pristine ZnIn2S4. The thin ZnIn2S4 nanosheet accelerates the separation of photogenerated electron pairs, and the amine groups on ZnIn2S4/NH–SiO2 act as active sites for adsorption and activation of CO2, hence facilitating the photoreduction of CO2.
研究领域:
材料科学
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环境科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2018
·Vol. 24
·期 34
·8596-8602
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IF 5.16
Yong Xu,Jiang Mo,Zi-Cheng Fu,Su Liu,Zhi Yang,Wen-Fu Fu
Graphical A hybrid photocatalyst consisting of Co and Co 2 P nanoparticles embedded in N, P-codoped carbon nanosheets was used in a visible light-driven system for CO 2 -to-CO conversion. The catalytic system displayed a high CO production rate of up to 35 000 μmol h −1 g −1 with CO selectivity of 79.1 % in the first 3 h of reaction. Linear CO production at an exceptionally high rate of 63 000 μmol h −1 g −1 was observed in the first 1 h of photocatalytic reaction. Artificial photosynthesis has attracted wide attention, particularly the development of efficient solar light-driven methods to reduce CO 2 to form energy-rich carbon-based products. Because CO 2 reduction is an uphill process with a large energy barrier, suitable catalysts are necessary to achieve this transformation. In addition, CO 2 adsorption on a catalyst and proton transfer to CO 2 are two important factors for the conversion reaction, and catalysts with high surface area and more active sites are required to improve the efficiency of CO 2 reduction. Here, a visible light-driven system for CO 2 -to-CO conversion is reported, which consists of a heterogeneous hybrid catalyst of Co and Co 2 P nanoparticles embedded in carbon nanolayers codoped with N and P (Co-Co 2 P@NPC) and a homogeneous Ru II -based complex photosensitizer. The average generation rate of CO of the system was up to 35 000 μmol h −1 g −1 with selectivity of 79.1 % in 3 h. Linear CO production at an exceptionally high rate of 63 000 μmol h −1 g −1 was observed in the first hour of reaction. Inspired by this highly active catalyst, Co@NC and Co 2 P@NPC materials were also synthesized and their structure, morphology, and catalytic properties for CO 2 photoreduction were explored. The results showed that the nanoparticle size, partially adsorbed H 2 O molecules on the catalyst surface, and the hybrid nature of the systems influenced their photocatalytic CO 2 reduction performance.
研究领域:
材料科学
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催化
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光化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 38
·2105001
·
IF 18.808
Yushuai Xu,Jian Han,Yidong Luo,Yaochun Liu,Junping Ding,Zhifang Zhou,Chan Liu,Mingchu Zou,Jinle Lan,Ce-wen Nan,Yuanhua Lin
Gaseous CO 2 reduction driven by solar energy is a promising solution to the current energy crisis and environmental problems. Although thermocatalysts, electrocatalysts, and photocatalysts are developed as classical strategies for CO 2 reduction, it remains a challenge for high efficiency and CO 2 net reduction during this process. Here, a multi-field driven hybrid catalyst, Pt/ZnO nanorod arrays/Bi 1-x Er x CuSeO, is designed using the photo-thermoelectric effect, which can take advantage of both photocatalysis and thermocatalysis. The results indicate that the maximum CO production rate of 2.91 µmol g −1 h −1 at 423 K can be realized in such Pt/ZnONR/Bi 0.9 Er 0.1 CuSeO hybrid catalyst, as can be ascribed to a synergetic photo-thermoelectric effect (i.e., light irradiation can provide heat, photo-excited carriers, and the concomitant Seebeck voltage). The band alignment of ZnO/BiCuSeO heterojunction and carriers transport are proposed to be optimized by the Er doped BiCuSeO thermoelectric supports, greatly enhancing the catalytic performance. The application of thermoelectric support could be promising in the structure design of multi-field driven hybrid catalysts, and such a photo-thermoelectric catalytic process demonstrates a desirable way of solar energy utilization in CO 2 transformation.
研究领域:
材料科学
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催化
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可再生能源
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环境科学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Mei Li,Zhenyang Zuo,Shengbo Zhang
Developing effective photocatalysts for CO2 reduction to high value-added chemicals or fuels is a promising strategy for alleviating serious environmental problems and energy crisis. Currently, the photocatalytic efficiency is still too slow to arouse industrial interest for most semiconductor photocatalysts due to their low CO2 uptake, limited visible light capture capacity, and serious recombination of electron–hole. Herein, we successfully synthesized a high-density ultrafine Au cluster (∼0.7 nm)-doped cobalt-layered double hydroxide nanocage (Au/Co-LDH) photocatalyst through an in situ redox strategy to explore the structure–activity relationship in the CO2 reduction system. A series of experimental characterizations showed that CO2 adsorption, visible light capture capacity, and charge transfer rate are significantly enhanced due to the highly dispersed and ultrafine Au cluster doping. Density functional theory calculations indicate that Au doping also promoted charge redistribution at the active site, increased the density of states near the Fermi energy level, stabilized the *COOH intermediate, and reduced the energy barrier of the rate-determining step. As a result, Au/Co-LDH delivers a CO evolution rate of 5610 μmol g–1 h–1 toward CO2 reduction under visible light (λ > 420 nm), which is 4 times and 22 times more active than the undoped one and Au nanoparticles, respectively. We believe that this work will provide an important implication for the development and optimization of photocatalysts for CO2 reduction.
研究领域:
材料科学
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环境科学
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化学工程
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纳米技术
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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）