SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Chao Du,Yunfei Ge,Junyi Qian,Zhijie Zhang
Solar-driven CO 2 conversion into reusable carbon forms is an attractive strategy to. reduce CO 2 emissions and provide feedstocks for industrial production. However, most of present catalysts suffer from poor light utilization and rapid charge recombination, thus severely restricting the efficiency of CO 2 photoreduction. Herein, an innovative strategy of integrating Cs 3 Bi 2 Br 9 and MnO 2 via self-assembly was established, with the aim of designing a multimodal photothermal catalyst for CO 2 reduction under full spectrum. In this hybrid, MnO 2 could combine with CBB to create an S-scheme photocatalyst with promoted carrier separation, and simultaneously acted as a “heater” to facilitate CO 2 photoreduction by effective photothermal conversion. Upon UV–vis-NIR illumination, the CBB/MnO 2 hybrid presented an impressively high CO production rate (R CO = 189.75μmol g −1 h −1 ). Theoretical calculations combined with experimental tests indicated that the excellent catalytic activity of CBB/MnO 2 could be ascribed to the synergetic effect of greatly increased carrier transfer and high photothermal conversion efficiency, resulting in considerably enhanced solar-light-driven photothermocatalysis with no extra heat input. The as-proposed catalyst in this study provides a novel and effective approach to develop highly efficient photothermal catalysts for solar-to-fuel applications.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
ACS Nano
·
2020
·
IF 14.588
Jianping Sheng,Ye He,Jieyuan Li,Chaowei Yuan,Hongwei Huang,Shengyao Wang,Yanjuan Sun,Zhiming Wang,Fan Dong
All-inorganic Pb-free bismuth (Bi) halogen perovskite quantum dots (PQDs) with distinct structural and photoelectric properties provide plenty of room for selective photoreduction of CO2. However, the efficient conversion of CO2-to-CO with high selectivity on Bi-based PQDs driven by solar light remains unachieved, and the precise reaction path/mechanism promoted by the surface halogen-associated active sites is still poorly understood. Herein, we screen a series of nontoxic and stable Cs3Bi2X9 (X = Cl, Br, I) PQDs for selective photocatalytic reduction of CO2-to-CO at the gas–solid interface. Among all the reported pure-phase PQDs, the as-synthesized Cs3Bi2Br9 PQDs exhibited the highest CO2-to-CO conversion efficiency generating 134.76 μmol g–1 of CO yield with 98.7% selectivity under AM 1.5G simulated solar illumination. The surface halogen-associated active sites and reaction intermediates were dynamically monitored and precisely unraveled based on in situ DRIFTS investigation. In combination with the DFT calculation, it was revealed that the surface Br sites allow for optimizing the coordination modes of surface-bound intermediate species and reducing the reaction energy of the rate-limiting step of COOH– intermediate formation from •CO2–. This work presents a mechanistic insight into the halogen-involved catalytic reaction mechanism in solar fuel production.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2018
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IF 4.439
Lu Li,Pan Li,Yanjie Wang,Lin Lin,Aamir Hassan Shah,Tao He
The defects like oxygen vacancy in a photocatalyst are critical factors to influence the photocatalytic reactivity since they can have an impact on the behavior of photogenerated charge carrier. Since oxygen vacancy can be readily formed in the ceria due to reversible conversion of the oxidation states between Ce 4+ and Ce 3+ , here ceria is used as the target material. A versatile and facile co-precipitation method was adopted to synthesize hydrangea-like Ce 1−x Zr x O 2 (x = 0.00, 0.025, 0.05 and 0.10). The amount of oxygen vacancy in the obtained catalysts can be modulated by altering the molar fraction of doped Zr. The composition, morphology, physico-chemical properties of the as-synthesized Ce 1−x Zr x O 2 were characterized by using different techniques. It is found that Zr doping into the ceria crystal lattice can lead not only to an enhanced specific surface area and surface adsorption capacity for CO 2 , but also to an increased concentration of oxygen vacancy that can exist in the bulk and on the surface. The Zr-doped ceria exhibits an enhanced activity for photoreduction of CO 2 , which can be explained based on the influence mechanism of oxygen vacancy. This work shows that the oxygen vacancy in the ceria can be modulated via a feasible Zr doping approach, which may help design the photocatalysts with high activity for CO 2 photoreduction.
研究领域:
材料科学
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化学
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环境科学
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催化
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 45
·16711-16719
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IF 4.39
Ying Jiang,Cunxin Mei,Zhijie Zhang,Zhongliang Dong
Perovskite CsPbBr3 nanocrystals (NCs) have emerged as promising candidates for the photocatalytic reduction of CO2. However, the CO2 conversion efficiency of pristine CsPbBr3 is still unsatisfactory, mainly due to severe radiative recombination, poor stability and low CO2 capturing ability. Coincidentally, nanoporous carbon powder (NCP) has received tremendous attention for environmental remediation and renewable energy production. Herein, by immobilizing CsPbBr3 NCs into the pores of NCP, a CsPbBr3/NCP hybrid has been successfully constructed for the first time, which combined the advantages of CsPbBr3 NCs and NCP. In comparison with pristine CsPbBr3, the resultant hybrid photocatalyst exhibited much superior photocatalytic performance in CO2 reduction, which could be attributed to the enhanced electron extraction and transfer between CsPbBr3 NCs and NCP, higher CO2 capturing ability and more active sites for CO2 activation. Furthermore, the nanohybrid displayed remarkable reusability in photocatalytic CO2 reduction. This study is anticipated to provide a new pathway for the design and fabrication of high-performance photocatalysts based on perovskites for solar-energy-conversion applications.
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
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Ganghua Zhou,Lirong Meng,Xin Ning,Weiqin Yin,Jianhua Hou,Qiao Xu,Jianjian Yi,Shengsen Wang,Xiaozhi Wang
Constructing type II heterojunction is an efficient strategy to enhance the light absorption and promote the charge transport. However, the improvement effect is limited by the decreased redox ability of charge carriers. The rational design of heterojunction from type II to Z-scheme is expected to overcome this obstacle. Herein, we demonstrate that the introduction of interfacial oxygen vacancies (OVs) can switch charge transfer of g-C 3 N 4 /BVO heterojunction from type II to Z-scheme. The interfacial OVs acted as the reactive center of charge carriers to quench the electrons of BVO and holes of g-C 3 N 4 , thereby promoting charge separation and migration. As a result, the interfacial OVs mediated Z-scheme g-C 3 N 4 /BVO heterojunction kept the strong oxidation/reduction potential of two single-component photocatalysts thereby significantly enhancing the photodegradation of tetracycline and CO 2 photoreduction. The kinetic constant of tetracycline degradation on the optimal g-C 3 N 4 /BVO-20 sample was 2.04-fold and 2.29-fold higher than those on g-C 3 N 4 nanosheets and pure BVO, respectively. This work provides a feasible strategy by the interfacial vacancy engineering of heterojunction for enhanced photocatalysis .
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Hongli Yang,Huilin Hou,Man Yang,Zhongli Zhu,Hui Fu,Dongdong Zhang,Yong Luo,Weiyou Yang
The selective photoreduction of CO 2 into hydrocarbon fuels, such as CH 4 , is highly desirable for sustainable energy but remains a significant challenge due to slow proton-electron transfer processes and competing intermediates. Herein, a novel NiO/MgAl-LDH (NMA-x, LDH represents layered double hydroxide) step-scheme (S-scheme) heterojunction has been engineered via in-situ anchoring MgAl-LDH nanoplates on metal–organic frameworks (MOFs) derived NiO microrods, which improves the CO 2 adsorption capability and specific surface area of NiO. The steered internal electric field in the p-n heterointerface promotes charge separation and attracts a high electron density center on the catalyst surface to favor CH 4 production. Meanwhile, S-scheme photogenerated charge transfer mechanism is proposed by in-situ X-ray photoelectron spectroscopy (XPS), in-situ diffuse reflectance infrared Fourier transform (DRIFT) spectra and density functional theory (DFT) calculation. In this process, photogenerated electrons are transferred from the conduction band (CB) of MgAl-LDH to the valence band (VB) of NiO, facilitating the CHO* species serve as the critical intermediate for producing CH 4 through desired photocatalytic CO 2 reduction. Using pure water as a proton source, the NMA-2 catalyst achieved a high CH 4 selectivity of 91.2% and a yield of 8.98 μmol∙g −1 ∙h −1 , representing significant potential for practical applications. This catalyst outperformed pristine and revitalized NiO by 4.23 and 2.07 times, respectively.
研究领域:
材料科学
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催化
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环境化学
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光化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
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IF 6.7
Changming Zhang,Yuan Wang,Xiaochao Zhang,Zhiyan Dong,Wensheng Wu,Caimei Fan
It is rather essential to increase CO 2 adsorption and improve separation efficiency of photoinduced carriers by solar-driven CO 2 reduction. Herein, we proposed a facile approach to synthesize millimeter-sized polyacrylonitrile-based carbon spheres (PANACSs) as a bifunctional adsorbent and self-nitrogen-doped source under a mild condition, and then embeds the highly active CeO 2 to construct a CeO 2 @PANACSs composite with strong adsorption capacity and high reduction activity. The involved XRD, XPS, SEM, N 2 adsorption/desorption, CO 2 adsorption, UV–vis DRS, EIS, PL and In situ FTIR spectra were characterized. Results suggested that the obtained PANACSs can act as a catalyst to drive the reduction of CO 2 into CO under visible light irradiation. CeO 2 @PANACSs showed the highest performance of photocatalytic reduction of CO 2 for 10 h (210.65 μmol·g −1 ), and the yield of CO evolution is approximately 1.83 times and 17.42 times higher than that of pristine CeO 2 and PANACSs, respectively. We found that the existence of nitrogen-containing functional groups further promoted the adsorption and activation of CO 2 . Among them, pyridinic nitrogen and pyrrolic nitrogen can be used as adsorption and activation sites to accelerate the separation and transfer of e - -h + . Furthermore, Ce 4+ on the surface of CeO 2 acts as an electron capture agent, which captures the electrons that are not transferred in time and reduces itself to Ce 3+ , and then the formed Ce 3+ reduces the adsorbed CO 2 to CO. Finally, the possible mechanism is proposed to depict the photocatalytic CO 2 reduction over the CeO 2 @PANACSs. Our finding provides a noteworthy promising strategy to construct bifunctional composite photocatalysts for achieving the high-efficient CO 2 adsorption and photoreduction to CO.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Mengying Tao,Zhaowei Jia,Hui He,Yanhu Han,Xin Yu,Yaofei Ren,Yuewei Wu,Yintong Lin,Zhongfeng Shi,Zhenxia Zhao,Zhongxing Zhao
Photocatalytic reduction of CO 2 exhibits unsatisfactory photocatalytic performance owing to the inefficient separation of photogenerated electron-hole pairs, low CO 2 capture efficiency and limited visible light absorption on most photo-catalysts. Herein, Ti F bridged IL-CuCQDs-F/TiO 2 inverse opal composite (IO-CFTi) was constructed for boosting CO 2 visible-photo reduction via slow photo effect. In this work, ethylenediaminetetraacetic acid (EDTA(Cu)) and imidazole ionic liquid 1-(2-Hydroxyethyl)-3-methylimidazolium tetrafluoroborate ([HOEtMIM][BF 4 ]) were employed to confine grow of IL-CuCQDs-F within TiO 2 inverse opal supporter via Ti F bonds connection. Unique IL-CuCQDs-F efficiently expended light absorption towards visible region, and the confined growth of IL-CuCQDs-F within the TiO 2 inverse opal cavity achieved the photoelectric conversion and efficient CO 2 capture. Moreover, their Ti F bonding interface of IO-CFTi assisted photogenerated electron transportation from TiO 2 to CO 2 for its reduction in this system. Consequently, IO-CFTi achieved a substantially increased CO production rate of 78.1 μmol·h −1 ·g −1 with 98 % selectivity. This improved performance in CO 2 photoreduction positions the nanocomposite as a promising material for preservation of the environment and conversion of energy.
研究领域:
环境科学
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材料科学
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光催化
✓ 已验证
DOI
PubMed
高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-10
·
IF 14.919
Sayed Mahmoud,Xu Feiyan,Kuang Panyong,Low Jingxiang,Wang Shengyao,Zhang Liuyang,Yu Jiaguo
Solar conversion of CO 2 into energy-rich products is one of the sustainable solutions to lessen the global energy shortage and environmental crisis. Pitifully, it is still challenging to attain reliable and affordable CO 2 conversion. Herein, we demonstrate a facile one-pot approach to design core-triple shell Mn, C-codoped ZnO hollow spheres as efficient photocatalysts for CO 2 reduction. The Mn ions, with switchable valence states, function as “ionized cocatalyst” to promote the CO 2 adsorption and light harvesting of the system. Besides, they can capture photogenerated electrons from the conduction band of ZnO and provide the electrons for CO 2 reduction. This process is continuous due to the switchable valence states of Mn ions. Benefiting from such unique features, the prepared photocatalysts demonstrated fairly good CO 2 conversion performance. This work is endeavoured to shed light on the role of ionized cocatalyst towards sustainable energy production.
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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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science China-Materials
·
2024
·Vol. 67
·期 2
·473-483
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IF 6.8
Guan Chen,Liao Yulong,Xiang Quanjun
Simultaneous optimization of surface and interlayer characteristics of graphite-phase carbon nitride (g-C 3 N 4 ) is crucial for enhanced photogenerated-carrier separation efficiency. Integration of distinct strategies with specific merits for constructing efficacious charge carrier transport pathways from bulk to surface faces challenges. Herein, we proposed a novel carboxyl functional group and potassium (K) ions co-modified g-C 3 N 4 for steering dynamic charge transfer processes. Specifically, carboxyl functional groups were grafted to the surface to substantially improve charge carrier dynamics through the driving force induced by its electron-withdrawing effects. Concurrently, K ions were inserted into the interlayers of g-C 3 N 4 to facilitate interlayer carrier transport by bridging adjacent layers. Such a bi-functional photocatalyst achieves 8.68-fold increase in CO yield compared wtih the pristine g-C 3 N 4 without any cocatalyst or sacrificial agent. This work provides a profound discernment into the directional transport of charge carriers within the surface and interlayers, and presents a promising approach for rational design of photocatalysts with remarkably efficient solar energy conversion.
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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纳米技术
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化学工程
✓ 已验证
DOI
高影响因子
Sustainable Energy & Fuels
·
2021
·Vol. 5
·期 14
·3598-3605
·
IF 6.367
Tangxi Chen,Min Zhou,Wen Chen,Yuyao Zhang,Siyong Ou,Yueli Liu
Halide perovskite quantum dots (HP QDs) have been widely used in the field of photocatalysis due to their excellent performance. However, the issues of lead toxicity and instability prevent their process in the photocatalysis application. Herein, the lead-free Cs2AgInCl6 perovskite quantum dots (CAIC QDs) are synthesized by the hot-injection method, and CAIC QDs@Ag composites with various Ag loading amounts are self-assembled by adjusting the Cl source in the synthesis process, which is used to improve the CO2 photoreduction efficiency by using the surface plasmon resonance (SPR) effect of Ag nanoparticles. In addition, the surface ligand density of CAIC QDs@Ag composites is regulated by the purification processing treatment to release the influence of organic ligands on the charge transport performance. It is found that the CAIC QDs@Ag composite with the optimal ligands density possesses fast electron transport and effective carrier separation efficiency, which are crucial for the improvement of the photocatalysis reaction. As a result, the CAIC QDs@Ag-2 composite after purification processing achieves the highest yield of 26.4 μmol g−1 and 28.9 μmol g−1 for CO and CH4, respectively, during the CO2 photoreduction process. In addition, there is no significant decline of CO2 photoreduction performance after the photocatalysis cycling test for 9 h, indicating the good stability of the CAIC QDs@Ag composite in the photocatalysis process.
研究领域:
材料科学
·
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Desen Zhou,Xuan Zhang,Zheng Li,Jun Zhang,Tielin Wang,Shaowen Cao
Photocatalytic conversion of CO 2 to usable fuels provides a new strategy for solving energy problems and the greenhouse effect. Porphyrin-based metal-organic frameworks (MOFs) are promising in photocatalysis due to their remarkable light harvesting ability, and the metal active site and its coordination environment can be further adjusted to achieve the high activity. In this work, g-C 3 N 4 /PCN-222 composites with different porphyrin metal centers were fabricated and the g-C 3 N 4 /PCN-222(Fe III ) catalyst showed the highest photocatalytic CO 2 reduction performance than that of g-C 3 N 4 /PCN-222(Fe II ) and other g-C 3 N 4 /PCN-222( M , M = Co, Ni, Cu, Zn) composites. Experimental studies and theoretical calculations showed that the axial coordination in g-C 3 N 4 /PCN-222(Fe III ) distorts the square planar field (Fe-N4) to quasi-octahedral coordination, which led to the moderate adsorption ability of CO 2 reduction intermediate (*CO), resulting in the high photocatalytic activity.
研究领域:
材料科学
·
环境科学
·
化学工程
·
催化
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）