Nanoscale
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2022
·Vol. 14
·期 42
·15889-15896
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IF 8.307
Yuxiang Ma,Yumin Zhang,Yiwen Ma,Tianping Lv,Bin Xiao,Xinya Kuang,Xiyu Deng,Jin Zhang,Jianhong Zhao,Qingju Liu
Single atom catalysts (SACs) have an extremely high atom utilization and distinctive structures and properties in the field of photocatalysis. However, the premise of conducting scientific research and applications is still the stability and catalytic activity of single atoms on suitable substrates. Metal organic frameworks (MOFs), as one of the most suitable single-atom substrates, have tunable internal structures, unsaturated coordination bonds, and high specific surface areas. In this work, Ti-based MOF, MIL-125, was adopted as the precursor to prepare mesoporous Cu-loaded TiO2. During the synthesis of MIL-125, a Cu source was added, and Cu atoms were fixed by partly replacing Ti atoms in the Ti–O octahedron to coordinate with O atoms, resulting in a good dispersity, good stability and high loading amount. Experimental investigations demonstrated that dispersed Cu single atoms act as reaction centres, besides being able to accelerate the transfer of photoelectrons. Under simulated sunlight, the H2 evolution rate of the optimum Cu–TiO2 sample reaches 17.77 mmol g−1 h−1, nearly 101 times higher than that of the pure mesoporous TiO2. The apparent quantum efficiency (AQE) is 20.15% under 365 nm irradiation. This research opens a new thinking to preparing high stability and high activity single atom photocatalysts.
研究领域:
材料科学
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光催化
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能源科学
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 31
·14879-14887
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IF 3.925
Fu Wang,Chunping Li,Tong Xu,Ying Li,Yinghui Sun,Jie Bai
Among rare earth oxides (REO), mixed-valence praseodymium oxide (Pr3+/Pr4+) has the highest O mobility and very promising applications in multiphase catalysis. In this paper, Pd-loaded praseodymium oxide nanotubes were successfully prepared by immobilizing Pd nanoparticles on modified carriers. XPS characterization showed that the electron transfer process during the reaction could be regulated by changing the Pr3+/Pr4+ ratio of praseodymium oxide. Importantly, the H2-PrxOy carrier surface has much higher Pd electron density, and the electron-rich Pd nanoparticles make it easier to break the C–Br bond and transfer electrons from Pd to C and Br atoms, leading to the formation of ArPdIIBr intermediate complexes. In the Suzuki coupling reaction, Pd/H2-PrxOy exhibited higher catalytic performance under mild conditions. There is a strong correlation between the surface properties of the carriers and the catalytic activity of the Pd nanocatalysts. This provides a new strategy for the preparation of Suzuki coupling reaction catalysts.
研究领域:
催化化学
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材料科学
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表面化学
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Ran Wang,Zhiding Zheng,Zhuo Li,Xiaoxiang Xu
Photocatalytic C-C coupling is a green and sustainable route to produce value-added chemicals. However, the product selectivity is generally non-tunable and there is a lack of an in-depth understanding of the dependence of product selectivity on the band structure of the semiconductor photocatalyst. Here, Zn x Cd 1-x S solid solutions have been explored for photocatalytic C-C coupling using benzyl alcohol as a typical reactant. The conversion rate of benzyl alcohol and selectivity of C-C coupling products is inherently linked to the solid solution level of Zn x Cd 1-x S which can be readily tuned. An optimal solid solution level has been found at Zn 0.6 Cd 0.4 S (x = 0.6) which delivers a conversion rate of 91.61% and a selectivity of 98.83% for C-C coupling products. These findings not only deepen the understanding on factors that affect product selectivity but also justify the usefulness of solid solutions in tuning the C-C coupling reactions.
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Journal of Materials Chemistry A
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2022
·Vol. 10
·期 34
·17668-17679
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IF 14.511
Zhengliang Zhao,Zhu Shu,Jun Zhou,Lina Ye,Tiantian Li,Wenbin Wang,Lina Xu
The efficiencies of visible-light utilization and exciton dissociation are crucial for the photocatalytic H2 evolution of poly(heptazine imide) (PHI), but simultaneously achieving both goals still presents a challenge. Herein, we firstly synthesized NH-rich red PHI nanoparticles (RPHI NP) with tunable n → π* electronic transition by calcining melamine using a KCl/KSCN molten system. The small particle size (about 50 nm in diameter) promotes charge separation via shortening the electron and hole transfer distance. Moreover, the n → π* electronic transition can be controllably regulated by changing the KSCN dosage, which remarkably broadens the optical response range to 750 nm. Collaborative optimization of the two enables RPHI1 NP to exhibit 25 times higher photocatalytic H2 evolution reaction (HER) rate than bulk PHI under visible-light irradiation (λ > 510 nm). This work details the simultaneous achievement of the optimization of charge separation and optical absorption of PHI via the synthesis of red PHI nanoparticles, which paves the way for developing advanced PHI materials.
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ACS Catalysis
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2021
·
IF 13.084
Zhiqiang Rao,Yuehan Cao,Zeai Huang,Zihang Yin,Wenchao Wan,Minzhi Ma,Yanxin Wu,Junbu Wang,Guidong Yang,Yi Cui,Zhongmiao Gong,Ying Zhou
Photothermal catalysis, which couples both solar and thermal energies, has burgeoned as a promising approach to drive catalytic reactions. However, the utilization of light irradiation to tune the reaction paths to obtain ideal product distribution in photothermal catalysis is still of tremendous challenge. Herein, we successfully regulated the relationship between two core competition reactions through light irradiation during photothermal dry reforming of methane over Ni/Ga2O3, resulting in the promotion of H2 formation and the suppression of the reverse water gas shift reaction. The increase in the H2/CO ratio from 0.55 to 0.94 could be achieved. Furthermore, the combination of density functional calculations and X-ray photoelectron spectroscopy reveals that light irradiation impelled the direction of electron transfer to be reversed from Ga2O3 to Ni to form the Ni0 sites, which provides the generation of abundant hot electrons from the electronic interband transition of Ni to boost the formation and desorption of H2. This work promotes the understanding of nonthermal behaviors of light irradiation in light-driven photochemistry, which is significant for designing catalysts with high efficiency and controllable product distribution.
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Journal of the Taiwan Institute of Chemical Engineers
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2019
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IF 3.834
Hang Jia,Xing-Rui Song,Sai Liu,Xia Xu,Xiu-Cheng Zheng,Zhi-Kun Peng,Pu Liu
As important multifunctional materials, the organic-inorganic hybrids are expected to be widely used in many fields, such as biosensor, solar cell and heterogeneous catalysis. In this article, we assemble a magnetic hybrid consisting of konjac glucomannan (KGM), graphene oxide (GO) and ferroferric oxide (Fe 3 O 4 ) via a co-precipitation method to anchor palladium nanoparticles . The resultant Pd/KGM-GO-Fe 3 O 4 catalysts exhibit superior catalytic performance for the hydrolysis of ammonia borane. The corresponding turnover frequency (TOF) is as high as 40.1 mo l H 2 mol Pd − 1 mi n − 1 in addition to a low activation energy ( E a = 26.1 kJ mol −1 ). The high catalytic activity is still maintained in the 10th recycle run, demonstrating their outstanding reusability. In addition, the magnetism of Fe 3 O 4 and the unique structure of the resultant catalysts achieve effective momentum transfer in an external magnetic field, endowing the easy separation of the catalysts from the reaction system with an external magnet. The results will facilitate the development of both H 2 generation and organic-inorganic hybrid-based materials.
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Journal of Materials Chemistry A
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2018
·Vol. 6
·期 24
·11337-11345
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IF 9.931
Wei-Ming Liao,Jian-Hua Zhang,Zheng Wang,Shao-Yun Yin,Mei Pan,Hai-Ping Wang,Cheng-Yong Su
Electron-deficient Ru/Rh half-sandwich units are optoelectronical, stereochemical, and redox and catalytically active in nature. Four different species of these units were designed and successfully incorporated into UiO-67 frameworks by post-synthetic exchange (PSE) method and employed for photocatalytic H2 evolution and CO2 reduction. Among them, the PSE-MOF catalysts containing [M–OH2] (M = Rh or Ru) groups show higher photocatalytic activity than those with [M–Cl], providing a new example of the exploitation of H2O molecules as small ancillary ligands for the construction of Ru/Rh half-sandwich units and subsequent incorporation into MOFs as photocatalytic centers. The application of TEOA (triethanolamine) and DMA (N,N-dimethylaniline) as sacrificial agents leads to different catalytic mechanisms and durations. A long-term hydrogen evolution lasting for 174 h without significant decrease in efficiency was achieved in the RhOH2@UiO-DMA system, showing the advantage of PSE-MOFs as highly stable photocatalytic platforms with superior self-protective properties.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2017
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IF 3.582
Ting Song,Piyong Zhang,Jian Zeng,Tingting Wang,Atif Ali,Heping Zeng
Metal-organic framework (MOF) materials with their synthetic tunability and structural regularity offer an interesting platform to achieve photocatalytic H 2 production. To determine whether metal ions in MOF materials affect the photocatalytic hydrogen (H 2 ) evolution activity, very few studies investigated MOF materials having the same crystal structures and ligands. In this study, we describe the synthesis of isostructural MOF materials. Cadmium (II) or copper (II) were linked with the 4′-(2,4-disulfophenyl)-3,2′:6′,3″-terpyridine (H 2 DSPTP) organic ligand to form Cd-MOFs and Cu-MOFs, respectively. Although Cd-MOFs and Cu-MOFs had the same valence band (VB) energy, the conduction band (CB) level of Cu-MOFs was more negative than that of Cd-MOFs. Therefore, the reduction ability of Cu-MOFs was greater than that of Cd-MOFs. Moreover, Cu-MOFs showed excellent absorption of visible and even near-infrared (NIR) radiation, because it has strong metal-to-ligand charge transfer (MLCT) character. Interestingly, the rate of photocatalytic H 2 generation was 18.96 μmol h −1 in the presence of Cu-MOFs, which were irradiated with NIR light ; however, Cd-MOFs did not report any such activity. Moreover, the performance and stability of Cd-MOFs were different from that of Cu-MOFs. In this study, the proof of knowledge for rational photocatalyst design introduced here furnishs the notional framework for constructing high-activity MOF materials.
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RSC Advances
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2016
·Vol. 6
·期 110
·108217-108228
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IF 3.289
Lujiang Xu,Zheng Han,Ying Zhang,Yao Fu
The vapor phase hydrodeoxygenation (HDO) of lignin-derived phenols under H2 atmosphere has great significance for producing high-quality fuels and commodity chemicals. Herein, we reported a simple, green method to prepare molybdenum oxide@N-doped carbon (MoOx@NC) via in situ pyrolysis of molybdenum precursor preloaded cellulose and demonstrated its catalytic performance for vapor phase HDO of lignin-derived phenols. When the pyrolysis temperature was at 600 °C, the catalyst (MoOx@NC-600) exhibited the best catalytic performance in vapor phase HDO of guaiacol. Through systematically investigating the parameters, such as: reaction temperature, WHSV, residence time, and concentration, the optimal reaction conditions for vapor phase HDO of guaiacol were 450 °C and 1 h−1 with atmospheric H2. The concentration of the feed was 20% in mesitylene, and the residence time was about 3.3 s. The carbon yield of aromatic hydrocarbons was 83.3%, with 65.7% benzene, 15.5% toluene and 2.1% alkylbenzenes. In addition, other lignin-derived phenols were also investigated and desired results were achieved with the MoOx@NC-600 catalyst. Furthermore, MoOx@NC-600 showed good stability due to the N-doped carbon formed on the surface of the MoOx particles. The catalysts were characterized using elemental analysis, AAS, BET, XRD, XPS, TEM, and EDS mapping. The high catalytic performance of MoOx@NC-600 toward lignin-derived phenols HDO can be attributed to the synergistic effect of the carbon supports and Mo5+ (molybdenum oxynitrides), Moδ+ (Mo2N) and Mo4+ on the surface of the MoOx particles.
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JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Huiting Lin,Yichang Ma,Xiaocan Wang,Guiqin Yi,Aimei Zhu,Qinglin Liu,Qiugen Zhang
Ether-free proton exchange membranes (PEMs) based on aromatic polymers are considered as potential alternatives to perfluorosulfonic acid (PFSA) PEMs due to their low cost, less reactant crossing, exceptional chemical stability and outstanding thermal stability. Herein, a series of high-performance sulfonated poly(biphenyl alkylene) (BPSA-PT- x ) membranes with full carbon chain backbones were synthesized to investigate the effect of different ratios of hydrophobic components on membrane properties. Among the prepared membranes, the BPSA-PT-10 % PEM with the highest proton conductivity (311 mS cm -1 at 80 °C water) possessed excellent dimensional stability (in-plane swelling rate ≤19.7 %, through-plane swelling rate ≤24.9 %), mechanical properties (elongation at break: 89.8 % in wet state), thermal stability (glass transition temperature >450 °C) and low H 2 crossover (1.80 mA cm -2 ). Further, the assembled H 2 /O 2 fuel cell based on BPSA-PT-10 % PEM exhibited competitive performance with a peak power density of 2.62 W cm -2 . The developed poly(biphenyl alkylene)-based PEMs should have potential applications in hydrogen energy field.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Yufeng Gan,Yuxiang Yang,Shunyan Ning,Yimin Liu,Yuezhou Wei,Xinpeng Wang,Deqian Zeng
Developing heterojunction photocatalysts is a critical method to augment the photocatalytic activity of single semiconductors. However, the instability of their heterostructure poses a significant challenge. Herein, a unique 0D/2D Mn 3 O 4 /CdS p-n photocatalyst has been prepared by a simple one-pot in-situ hydrothermal approach for H 2 production and methylene blue (MB) degradation. The optimized MC-0.18 (18 at% Mn) nanocomposite showed remarkable photocatalytic properties, producing a significantly higher H 2 generation rate of 1291 μmol· g −1 · h −1 , which was 13.7 and 9.2 times higher than that of pristine CdS and ex-situ synthesized MC-0.18-ex photocatalysts, respectively. MC-0.18 displayed the highest reaction rate at 0.0435 min −1 for MB degradation, which was approximately 2.6 and 6.3 times higher than CdS and Mn 3 O 4 , respectively. Active species capture experiments and ESR identified •OH and •O 2 − as the main substances involved in MB degradation. Importantly, MC-0.18 demonstrated excellent stability and reusability in photocatalytic H 2 production and MB degradation cycle tests. The formation of unique p-n heterostructures results in enhanced photoactivity due to the matched band alignment between ultrafine Mn 3 O 4 nanoparticles and CdS nanosheets , leading to a high charge separation capacity. This study offers a facile route to design p-n heterojunctions that have remarkable charge transfer abilities to promote H 2 production and degrade organic dyes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Xinyi Zhang,Yinxiang Chen,Rongshuo Guo,Zhijun Zhang,Zhe Sun,Ye Zhang,Feng Yan
Ionic liquids (ILs) have emerged as new persistent pollutants in aquatic environments due to their notable ecotoxicity. Herein, In 2 Se 3 @Ag 3 PO 4 S-scheme piezo-photocatalyst with interfacial In-O and Se-P covalent bonds is prepared for efficient degradation of 1-butyl-2,3-dimethylimidazole bromide ([BMMIm]Br). The experimental results demonstrate that 98.3 % of [BMMIm]Br is degraded under piezo-photocatalysis. Notably, [BMMIm]Br functions as a hole sacrificial agent, leading to a simultaneous H 2 production rate of 582.7 μmol g −1 h −1 and a co-removal efficiency of 97.2 % for radioactive heavy metal ions of U(VI), achieving the "three birds with one stone" effect. Density functional theory (DFT) calculations indicate that the S-scheme structure, combined with the In-O and Se-P covalent bonds and the piezoelectric effect, effectively promotes the separation of electron/hole pairs while inhibiting carrier recombination dynamics, thereby enhancing piezo-photocatalytic performance. Moreover, systemic toxicity evaluations, including assessments of calculated toxicity, zebrafish growth, and bean sprout development, were conducted to verify the reduced toxicity of the degraded intermediates, highlighting the potential practical applications of this approach.
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