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
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
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2018
·Vol. 148
·期 9
·2799-2811
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IF 2.911
Huang Qifu,Li Wenzhi,Lei Yanyan,Guan Shengnan,Zheng Xusheng,Pan Yang,Wen Wu,Zhu Junfa,Zhang Haitao,Lin Qizhao
Abstract In this work, NiCo 2 O 4 with a hierarchical porous flower-like structure was fabricated and used as catalyst support for Pd nanoparticles. The NiCo 2 O 4 was composed of porous nanoplates without overlapping, and the Pd nanoparticles were uniformly distributed on these nanoplates. Pd–NiCo 2 O 4 with the Pd loading of 2.0 wt% showed extremely high activity and stability, methane (1.0% CH 4 /Air) can be totally oxidized at 330 °C and the T 90 is 309 °C, which is much lower than that of pure NiCo 2 O 4 (T 90 = 405 °C). At wet condition with the presence of 10 vol% water vapor, the catalytic activity was still acceptable with the T 90 of 366 °C, and no activity decrease or permanent damage for the catalyst was observed after 35 h reaction, showing high stability. A series of techniques including TEM, SEM, XRD, H 2 -TPR, BET and especially quasi in situ XPS combined with in situ MS were used to characterize the catalysts and investigate the catalysis mechanism. Two pathways of CHO evolution were proved by the quasi in situ XPS and in situ MS results: OCHO intermediate dehydrogenation pathway at lower temperature and CO oxidation pathway of CHO at higher temperature. Graphical Abstract
研究领域:
化学
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材料科学
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催化
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环境科学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Ying Zhang,Jiaqi Yang,Kai Wei,Yulu Xue,Liying Cai,Huarui Han,Changchang Ma,Sheng Feng
The thoughtful construction of highly efficient, tiered photocatalysts has become a focal point of interest. Herein, in this context, the step-scheme (S-scheme) AlBi-MOF/MgNiAl-LDH heterojunction is specifically engineered to facilitate the photocatalytic reduction of CO 2 . The CO 2 photocatalytic reduction experiments of three samples, AlBi-MOF, MgNiAl-LDH and AlBi-MOF/MgNiAl-LDH, were conducted for 5 h using triethanolamine as the sacrificial agent, the optimized sample demonstrates significantly enhanced CO 2 photoreduction efficiency compared to the control without treatment, i.e., AlBi-MOF and MgNiAl-LDH. The optimized AlBi-MOF/MgNiAl-LDH exhibited a CO 2 reduction rate of 86.84 μmol g −1 h −1 , which was 25.85 times higher than that of MgNiAl-LDH alone and 20.15 times higher than that of AlBi-MOF alone. The improved photocatalytic efficiency is mainly attributed to the decreased recombination of photogenerated charge carriers, facilitated by S-scheme heterojunction. Additionally, the large specific surface areas and abundant active sites also contribute to the improvement. Meanwhile, the S-scheme photocarrier transfer mechanism was verified by in situ X-ray photoelectron spectrum (XPS) and femtosecond transient absorption spectroscopy (fs-TA). This research outlines an effective methodological for advancing highly efficient heterojunction photocatalysts dedicated to the transformation of solar energy into fuel.
研究领域:
材料科学
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纳米技术
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环境科学
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能量转换
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物理化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
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2024
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IF 6.7
Gongcheng Sun,Wan Chen,Yaoying Li,Subing Fan,Junmin Lv,Tiansheng Zhao
The hydroformylation reaction is very important in industry. However, the leaching of the noble metal Rhodium (Rh) and the separation of homogeneous catalyst have always been difficult problems to solve. And even heterogeneous Rh-base catalyst was developed to solve the separation problem, the serious Rh losing is still hard to avoid. In this work, heterogeneous encapsulated Rh@NaX was prepared by using one-step synthesis method and used as catalyst without reduction in 1-hexene hydroformylation reaction. Rh@NaX catalyst exhibited outstanding catalytic performance. When directly complexed with ligand triphenylphosphine (PPh 3 ), it achieved high heptanal yield of 97.53 %, high n/i ratio of 2.59 and high TOF of 6588 h −1 . Interestingly, encapsulated catalyst exhibited higher recycling stability and much lower Rh leaching compared to impregnated catalyst. In addition, in situ XPS and DRIFT analyses were conducted to elucidate the reduction process of Rh and the reaction pathway.
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
DOI
高影响因子
Nanoscale
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2023
·Vol. 15
·期 39
·16131-16143
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IF 6.7
Jingzhi Wang,Mei Li,Zhiliang Jin
Dynamics and morphology play a crucial role in the field of photocatalytic hydrogen production. Regulating the transfer of photogenerated charges is an effective way to improve the catalytic activity. In this paper, 1T-WS2 is introduced into a p–n heterostructure, ZnCdS/NiV-LDH, as a metalloid electron pump to transfer photogenerated electrons from semiconductors with larger work functions to metalloid materials with smaller work functions, effectively to attract photogenerated electrons, and promote charge rearrangement at the p–n heterostructure interface, so as to achieve the best utilization efficiency of photogenerated charges. Second, adjusting the morphology to increase the light absorption area of the catalyst is also a way to improve the photocatalytic activity. Two different nanosheet structures dispersed heavily stacked ZnCdS, increasing the light absorption area of the system. The optimal catalyst ratio achieves a hydrogen evolution rate of 22.37 mmol g−1 h−1, achieving 7.98% AQE and 2.12% STH conversion efficiency at 450 nm. The potential mechanism was demonstrated through in situ XPS. This study provides new insights into adding “electron pumps” to heterostructures to enhance photocatalytic activity.
研究领域:
材料科学
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催化
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纳米技术
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光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
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2025
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IF 13.1
Rui Zhai,Zhenyu Wang,Chang Huang,Chao Zeng,Mengyue Gu,Tianqi Wang,Fanqi Bu,Shaobin Wang,Jinying Zhang
Phosphorus has various crystallographic structures and variable phosphorus-derived structures, which have attracted much attention due to its unique properties. One-dimensional phosphorus structures with atomic substitution in the phosphorus lattice are extremely favored due to their high specific surface area and stable single-atom dispersion. The precise crystal structures and single atomic substitution positions are crucial factors to understand the mechanism of single-atom effects but remain a big challenge. Herein, single crystals composed of 1D zigzag linear phosphorus selenium chains (ZLP-Se) have been produced and characterized by SC-XRD to be P18.56Se1.44 with a space group of Pnma (CSD-2348033). The exact Se substitution positions were further ascertained by calculations of the whole thermodynamic stability phase diagram to have three types of substitution patterns (Se1/P1 mixed occupied positions with intervals of 3Se+2P, 1Se+4P, and 1Se+1P+1Se+2P). The selenium-rich crystal plane (-10-1) has been demonstrated to significantly enhance CO2 adsorption and C−C coupling to obtain ethylene (C2H4). A high photocatalytic CO2 reduction performance (18.0 μmol g−1 h−1, 97.0% electron selectivity for C2H4) has been achieved by the ZLP-Se with the Ag cocatalyst. The adsorption of CO2* and CO* was found to be much stronger on the Se-rich surface of ZLP-Se. The CO* intermediates were found to be energetically favored for protonation and subsequent asymmetrical C−C coupling to produce C2H4, with COCHO* intermediates detected by in situ DRIFTS. The electron was also demonstrated by in situ XPS to transfer from Se and Ag to P under Xe lamp irradiation, confirming the electronic localization effect of ZLP-Se to yield C2H4.
研究领域:
材料科学
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催化
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物理化学
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纳米技术
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环境科学
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产品关联
DOI
高影响因子
ADVANCED MATERIALS
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2025
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IF 26.8
Zailun Liu,Yunfei Ma,Junqing Li,Ying Tu,Hui Yang,Kelin He,Chao Chen,Yulin Wang,Xiang Lin,Hongli Sun,Chenliang Su,Qitao Zhang
Uncovering the excitation processes of photocatalysts and enhancing the dissociation of excitons into free photogenerated electrons and holes for photocatalytic CO 2 reduction is imperative yet quite challenging. Herein, an efficient strategy of reducing the binding energy of excitons to boost exciton dissociation is reported by anchoring the low valence single-atom Cu sites in In 2 S 3 nanosheets (Cu-In 2 S 3 ), which can enhance photocatalytic CO 2 reduction activity. The investigations of photo-irradiated Kelvin probe force microscopy (KPFM), in situ irradiates X-ray photoelectron spectroscopy (XPS), and temperature-dependent photoluminescence (TD-PL) indicate that the doping of low valence single-atom Cu can efficiently drive the charge transfer and separation. Moreover, the studies of the dynamic behaviors of charge carriers by femtosecond time-resolved spectroscopy (fs-TAS) reveal that the doping of low valence Cu single-atom sites allows the promotion of exciton dissociation by reducing the binding energy of the exciton, resulting in an enhanced photocatalytic CO 2 reduction of Cu-In 2 S 3 nanosheets. The aforementioned strategy for enhancing the dissociation efficiency of excitons in photocatalysts will offer a highly efficient and promising approach for the photocatalytic CO 2 reduction and other photocatalytic applications.
研究领域:
光催化
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材料科学
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纳米技术
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物理化学
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能量转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Chaogang Ban,Yang Wang,Jiangping Ma,Yajie Feng,Junjie Ding,Youyu Duan,Xue Liu,Bin Zhang,Jinjing Tang,Xiaoping Tao,Liyong Gan,Shuangshuang Tan,Xiaoyuan Zhou
Rational fabricating advanced photocatalysts to recycle CO 2 into solar fuel is one of the most promising approaches to simultaneously address energy shortages and global warming. TiO 2 has been widely used in photocatalytic CO 2 reduction due to its abundant reserves, non-toxicity and harmlessness etc. However, it remains significantly challenging for practical applications due to the fast electron-hole recombination. Herein, we design a direct TiO 2 based Z-Scheme heterojunction by self-assembly of C-doped TiO 2 nanoparticles on 3D hierarchical petal of flower-like β-Bi 2 O 3 (C-TiO 2 /β-Bi 2 O 3 ). In situ electron paramagnetic resonance tests, in situ X-ray photoelectron spectroscopy and theoretical calculations reveal that electrons are transferred from β-Bi 2 O 3 to C-TiO 2 due to the formation of Z-Scheme heterojunction, which greatly accelerates the separation of photogenerated carriers to promote efficient CO 2 photoreduction. Ultimately, the optimal heterojunction shows significantly enhanced photocatalytic activity for CO 2 reduction to CO (31.07 μmol g –1 h −1 ) compared to the pure TiO 2 (3.28 μmol g –1 h −1 ) without using any photosensitizers and sacrificial agents. This work provides a unique insight to design direct Z-Scheme heterojunctions and delivers a promising photocatalyst for overcoming global warming and energy-supply issues.
研究领域:
材料科学
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环境科学
·
化学工程
·
光催化
✓ 已验证
DOI
高影响因子
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