MICROPOROUS AND MESOPOROUS MATERIALS
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2021
·
IF 5.455
Meng Rong,Liangrong Yang,Chao Yang,Jiemiao Yu,Huizhou Liu
Herein, a new tetraphenyladamantane-cored triazine-based multiamine (TPADT) was designed and synthesized. Its bulky molecular volume, strong rigidity, and high amine functionality enable it easy to prop up the polymer backbone and form a high hypercrosslinking degree to obtain high microporosity. A series of highly microporous tetraphenyladamantane-based polyaminals (Ad-MALPs) were prepared through the catalyst-free copolymerization of TPADT and commercial aromatic aldehydes. By changing the strut length and functionality of aldehyde monomers , the resulting polymers exhibit tailored BET surface area (1541–1779 m 2 /g) and narrow ultramicropore size distribution (0.52–0.93 nm). Ad-MALP-2 with the largest microporosity possesses the highest CO 2 uptake (21.1 wt %, 273 K/1.0 bar) and CO 2 /N 2 adsorption selectivity (35.2). Interestingly, Ad-MALP-3 shows the highest H 2 uptake (2.26 wt%, 77 K/1.0 bar) due to larger total pore volume . In addition, highly microporous Ad-MALPs simultaneously contain aromatic and cycloaliphatic components, and thus show exceptionally large aromatic and cycloaliphatic organic vapor adsorption capacity under low pressure. At P/P 0 = 0.1, the benzene and cyclohexane vapor uptakes of Ad-MALPs are up to 44.8 wt% and 39.0 wt %, far exceeding that of most previously reported porous organic polymers . Considering that Ad-MALPs have outstanding gas adsorption performance, simple preparation, good stability, and cycle ability, they are expected to be promising adsorbent materials for CO 2 adsorption/separation, H 2 storage and low-concentration volatile organic vapors capture.
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2021
·Vol. 32
·期 4
·4125-4131
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IF 2.478
Zheng Han,Liu Ying
Cu 2 ZnSnS 4 (CZTS), with a direct bandgap of 1.5 eV, is a primary candidate material for solar energy conversion applied in both photovoltaics and photocatalysis due to its tremendous reserves and environmental friendly components. Though the utilization of CZTS with phases of kesterite and wurtzite are extensive, until now, the synthesis and growth procedure of both phases are not clearly understood. In this work, we succeed in synthesizing CZTS microspheres with controlled phase through a facile method—ultrasonic spray pyrolysis (USP). By choosing ammonium thioglycolate and l -cysteine as sulfur source, which were found to be the key factor in the phase formation process, CZTS microspheres can be prepared in kesterite phase and wurtzite phase, respectively. After exposing the prepared CZTS microspheres under the Xe lamp irradiation, we found an apparently phase-dependent photocatalytic hydrogen evolution, in which the performance of kesterite phase CZTS sample was almost 2 times as high as that of wurtzite CZTS sample.
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CERAMICS INTERNATIONAL
·
2020
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IF 3.83
Song Liu,Jinxing Huang,Haiwei Su,Guogang Tang,Qinqin Liu,Jingfang Sun,Jing Xu
Constructing appropriate cocatalysts to modify semiconductors is significant for improving photocatalytic H 2 production and stability. Transition metal phosphides (TMPs) with low-cost and high efficiency have been considered as one of the most promising non-noble-metal cocatalysts. Herein, a novel multiphase phosphide nanosheet , Fe 2 P/Ni 3 P cocatalyst, was target designed and in-situ incorporated with Cu 2 O nanocubes via a phosphorization method for photocatalytic H2 evolution under visible light irradiation. The optimal Cu 2 O/Fe 2 P/Ni 3 P sample provided 10-folds higher photocatalytic activity of H2 evolution rate (108.68 μmol g−1 h−1) than that of single Cu 2 O (18.6 μmol g −1 h −1 ), which could be ascribed to fast charge transfer from the Cu 2 O to multiphase phosphide Fe 2 P/Ni 3 P cocatalyst and efficient separation of the light-induced charge carriers. Moreover, the Fe 2 P/Ni 3 P cocatalyst also improved the photo-corrosion of Cu 2 O caused by the disproportionation reaction, leading the Cu 2 O/Fe 2 P/Ni 3 P hybrid possessed robust stability. Additionally, this work guarantees useful insights in employing novel TMPs-based cocatalysts to construct visible-light-responsive photocatalysts , which manifests promising applications in the dwindling supply of energy.
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Materials Chemistry Frontiers
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2020
·Vol. 4
·期 6
·1671-1678
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IF 6.788
Ping She,Jun-sheng Qin,Heng Rao,Buyuan Guan,Jihong Yu
Efficient charge separation and light harvesting of photocatalysts (e.g., TiO2) are the key issues to be considered in the design of solar-energy conversion systems. In particular, the charge separation of noble metal-decorated TiO2 materials could be greatly improved via decreasing the size of noble metal particles (NPs). Furthermore, designing specific morphologies such as hollow structures can improve light harvesting ability. Herein, a hybrid hollow TiO2 with spatially separated bimetals (Pd@TiO2@Au) was prepared, which demonstrated enhanced charge separation. By choosing zeolite as the sacrificial substrate, ultrasmall Pd NPs and Au NPs were decorated in the inner and outer shells of hollow TiO2, respectively. The separated bimetals could pull the photoexcited electrons away from the surface of TiO2 for more efficient charge separation. The as-prepared Pd@TiO2@Au catalyst exhibited a superior photocatalytic H2 evolution rate up to 272.3 μmol h−1, which was higher than most of the TiO2-based photocatalysts.
研究领域:
材料科学
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光催化
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太阳能转换
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高影响因子
FUEL PROCESSING TECHNOLOGY
·
2019
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IF 4.507
Xiaoping Wu,Qiao Zhang,Lungang Chen,Qiying Liu,Xinghua Zhang,Qi Zhang,Longlong Ma,Chenguang Wang
The development of thermally stable Pt-based catalysts with superior performance for propane dehydrogenation reactions remains a daunting challenge. In this study, a series of PtSn-Mg(Zn)AlO catalysts with different Zn and Pt contents were synthesized by the anion-exchange method for the propane dehydrogenation reaction. To investigate the influence of Zn on the reaction performance and the catalyst structure, the prepared catalysts were characterized with several analytical techniques, including XRD , TEM, HRTEM, H 2 -TPD and CO pulse chemisorption . A good propane conversion (initially higher than 55% and averaging 45.2% over a period of 2 h) and propene selectivity (higher than 99%) were obtained experimentally with PtSn-Mg(3Zn)AlO at 550 °C. The results demonstrated that Pt provided the active sites and that Zn was a promoter. The HRTEM and CO pulse chemisorption results indicated that the addition of Zn to the PtSn-MgAlO catalyst can stabilize the dispersion of metal particles and thus inhibit the sintering of Pt particles. Furthermore, the activities of the used catalysts were almost recovered through reaction-regeneration cycles with the burning-off of coke during five cycles.
研究领域:
催化
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化工
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材料科学
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高影响因子
Journal of Materials Chemistry C
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2024
·Vol. 12
·期 22
·8145-8152
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IF 5.7
Dongkai Hu,Mavlanjan Rahman,Shuifu Liu,Lina Shen,Pengpeng Dai,Dawei Wen,Mingmei Wu
While numerous approaches have been devised to optimize the luminescence properties of Eu2+-activated phosphors, the quest for a simple design strategy to achieve color-tunable Eu2+ emission remains a significant challenge. Here, we present a straightforward, doping-free method to tailor the site occupation of Eu2+ and modify its luminescence properties. In the pristine sample, the NaBaB9O15 (NBB) host featuring two cation sites (Na+ and Ba2+), Eu2+ exclusively occupies the Ba2+ site, resulting in blue emission when the NBB:Eu2+ phosphor is synthesized in a H2 reducing atmosphere. When we use CO instead of a H2 reducing atmosphere, impressively, the formation energy required for heterovalent substitution of Na+ by Eu2+ is lowered, leading to the emergence of a distinct green emission band. Significantly, the resultant phosphor NBB:Eu2+@CO exhibits not only a high internal quantum yield of 85.1% and zero-thermal-quenching behavior within the temperature range of 25–200 °C but also wavelength-tunable emission. Benefitting from the multi-color luminescence of the NBB:Eu2+@CO phosphor, its optical applications will no longer be confined to general lighting but extend to anti-counterfeiting and encryption. This study provides a novel design methodology for optimizing the optical properties of Eu2+-activated phosphors.
研究领域:
材料科学
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光学
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化学
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高影响因子
CHEMICAL PAPERS
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2024
·Vol. 78
·期 4
·2275-2285
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IF 2.1
Shu Ronglu,Du Yifan,Cao Liping,Zhao Hui,Luo Xiaoying,Wang Wei
Cerium samarium oxides catalysts with K + doping on the wall surface of cordierite honeycomb ceramics were preparation by sol–gel and dipping processes. Scanning electron microscopy, energy dispersive X-ray spectroscopy, X-ray diffraction and Fourier transform-infrared spectroscopy were used to characterize the structural morphology and phase compositions. Through XPS analysis and H 2 -TPR measurement of monolithic catalyst, it is found that potassium ions improve the oxygen mobility in CeO 2 lattice and form surface active oxygen, increase the amount of oxygen adsorbed on the surface and improve the oxidation–reduction capacity. The catalytic combustion research demonstrates that T 10 , T 50 and T m in samples (Ce/Sm-0 K, Ce/Sm-0.3 K, Ce/Sm-0.5 K and Ce/Sm-0.7 K) decrease significantly compared with the blank reference (Cordierite). And the optimized sample Ce/Sm-0.5 K possess the lowest T 10 (389.6 °C), the lowest T 50 (425.5 °C), and the lowest T m (419 °C) in comparison with other samples. The cycle stability investigation reveals that sample Ce/Sm-0.5 K has excellent structural stability and stable catalytic performance, which has potential application in soot catalytic combustion field.
研究领域:
催化化学
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材料科学
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环境工程
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化学工程
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表面科学
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高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Shenghan Gao,Yuting Luo,Bo Li,Wen Cai,Huai Liu,Rui Zhang,Wenlong Jia,Lincai Peng
Modulating the electronic environment of single-atom metal catalysts is a promising yet challenging strategy to optimize their catalytic performance. Herein, electron-rich Ru single atoms were successfully confined within a CoOx matrix (Ru0.6CoOx) through a simple manual grinding-reduction strategy. The resulting Ru0.6CoOx catalyst demonstrated exceptional catalytic activity for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF), affording a nearly quantitative DMF yield with an impressive DMF productivity of 210.2 molDMF·mol–1Ru·h–1 at 160 °C. This productivity outperforms most of the noble metal-based catalysts for DMF production. Notably, Ru0.6CoOx also enabled the efficient conversion of HMF to DMF at a low reaction temperature of 120 °C or using a concentrated HMF solution (up to 20 wt %). Experimental studies combined with density functional theory calculations (DFT) revealed that the electronic interaction between the Ru species and CoOx generates electron-rich Ru single atoms, which serve as active sites to boost the H2 activation. Furthermore, the introduction of single Ru atoms was shown to increase the acidity of Ru0.6CoOx, thereby facilitating the cleavage of the C–OH bond during HMF hydrogenolysis. The boosted H2 activation ability and improved acidity of Ru0.6CoOx contribute significantly to its outstanding catalytic performance. This work provides valuable insights into the preparation of electron-rich single-atom metal catalysts for the catalytic hydrodeoxygenation of biomass-derived chemicals.
研究领域:
催化化学
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材料科学
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化学工程
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生物质转化
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密度泛函理论(DFT)
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2014
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IF 6.007
Moa Z. Granlund,Kjell Jansson,Marita Nilsson,Jazaer Dawody,Lars J. Pettersson
The objective of this paper was to study the influence three promoters (Co, La, Mn) had on the catalytic activity of Rh-based catalysts for autothermal reforming of diesel. The catalysts were supported on CeO 2 -ZrO 2 and the loading was 1 wt.% Rh and 6 wt.% promoter. The catalytic activity was evaluated in a monolith bench scale reactor with Swedish Environmental diesel, MK1. The process parameters employed at the ATR experiments were; O 2 /C ∼ 0.45, H 2 O/C ∼ 2.5 and GHSV ∼ 50,000 h −1 , meanwhile the reactor temperature was ramped from 700 °C to 950 °C. The catalysts were compared based on their fuel conversion, H 2 yield and the selectivity of different short-chain hydrocarbons. The results showed that all three catalysts had both high fuel conversion and H 2 yield in the optimal ATR operation temperatures. The H 2 yield and fuel conversion were increasing in the order Rh/Mn, Rh/La, Rh/Co. To get further insight in the difference between the materials the fresh and aged catalytic materials were characterized. The characterization methods used were H 2 -temperature programmed reduction (H 2 -TPR), powder X-ray diffraction (XRD), and BET surface measurements. The BET surface measurements showed that promotion with La gave improved thermal stability of the material. The XRD showed a high dispersion of all metals except Co, which was present as crystals in the size range of the particles of the support.
研究领域:
催化
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化学工程
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环境科学
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Jagadeesh Suriyaprakash,Abdul Khader Jilani Saudagar,Lijun Wu,Lianwei Shan
A key challenge in renewable energy is achieving cost-effective, industrial-scale hydrogen production through water splitting, which necessitates highly efficient epitaxial heterojunction photoelectrodes. However, current fabrication methods fail to provide advanced materials with the essential trifecta of flexibility, durability, and energy efficiency, which are crucial for next-generation energy systems. Herein, we present machine learning (ML)-powered laser-writing fabrication parameters to engineer laser-induced graphene-Cu 2 O (bottom) /CuO (middle) /anisotropic carbon (top) [hereafter Cu 2 O/CuO/LIAC] heterostructures, merging ML with nanoscale precision. Using Bayesian optimization of 11 laser parameters (trained on physics-informed data), we achieve sub-3 % thickness control (0.18–2.11 % deviation) for epitaxial heterostructures, while gradient-boosted regression identifies laser-carbonization kinetics as the critical stability determinant. The resulting Cu 2 O/CuO/LIAC photocathode, comprising a current-collecting LIG layer, photoactive Cu 2 O/CuO bilayer, and anticorrosion/active electrolyte interface layer, exhibits exceptional performance: −3.2 mA cm −2 photocurrent (0 V vs. RHE) and 0.373 mmol g −1 h −1 H 2 yield under solar irradiation. Notably, it maintains ∼88 % photocurrent after 3000+ bending cycles (r = 5 mm), paired with robust recyclability and electrolyte stability. This ML-accelerated approach reduces optimization costs by 47 % versus trial-and-error methods, enabling scalable fabrication of flexible, stable heterostructures. By bridging AI-driven process control with laser precision, we advance next-generation photoelectrodes for sustainable H 2 energy.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Kaixuan Feng,Ruixiang Lin,Yuyan Hu,Yuheng Feng,Dezhen Chen,Tongcheng Cao
Hydrogen-based selective catalytic reduction (H 2 -SCR) is gaining attention for its environmental benefits, in response to increasingly stringent global N 2 O emission regulations. This study investigates the catalytic performance of alkali metal-activated char (K, Ca, Na) in reducing N 2 O using H 2 at temperatures below 200℃, through theoretical calculations and experimental validation. The study reveals that K, Na, and Ca exhibit distinct behaviors in terms of loading sites. K and Na preferentially decorates at edge sites due to differences in electron conjugation and atomic population, while Ca is more inclined to load at central positions, forming strong interactions with the char. These differences lead to variations in the N 2 O reduction pathways: K/Na-char primarily engages in physical adsorption, with N 2 O reduction proceeding through higher energy barriers, whereas Ca-char facilitates chemical adsorption of N 2 O with minimal energy barriers, displaying significant catalytic activity, Despite these differences, the study identifies a common rate-determining step across all systems, predominantly involving the removal of H 2 O. Notably, Ca-char achieves a substantial reduction in activation energy to 42.1 kJ/mol, compared to the partial reduction achieved by K/Na-char to 165.4–178.3 kJ/mol, from an initial 383 kJ/mol. Experimental validation corroborates the catalytic performance of all three alkali metals.
研究领域:
环境化学
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催化
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材料科学
·
理论与应用化学
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Yuehu Wan,Shiwen Du,Congrong Lu,Kuankuan Ren,Biyun Shi,Shiyan Liu,Chunhe Li,Weidong Dou,Ping Fang,Na Ye
Visible-light-driven photocatalysis holds a broad prospect for alleviating the energy crises. Here we report novel CuS nanoparticles/CdS nanowires Schottky heterojunctions via a two-step hydrothermal synthesis and used for photocatalytic H 2 generation driven by visible-light (λ ≥ 420 nm). Compared with pure CdS NWs, the CuS/CdS nanocomposites show outstanding visible light H 2 evolution, with an optimal rate reaching 2076.5 μmol h −1 g −1 . The intrinsic properties of CuS/CdS nanocomposites, such as structure, optical properties , and combined configuration are systematically analyzed by experimental characterizations and theoretical calculations. The comprehensive results show that the Schottky junction between CuS NPs and CdS NWs accelerates photoinduced electron drift from semi-conductive CdS to metallic CuS, improving their activities of water splitting. This work offers a simple route to synthesize one-dimensional CdS-based nanocomposites for efficient visible-light driven energy conversion.
研究领域:
材料科学
·
能源科学
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