RSC Advances
·
2023
·Vol. 13
·期 13
·8915-8922
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IF 3.9
Tong Zhou,Haitang Wei,Bin Xiao,Tianping Lv,Liangfei Duan,Qingjie Lu,Jin Zhang,Yumin Zhang,Qingju Liu
One of the most promising strategies for producing hydrogen is photocatalytic water splitting, in which the photocatalyst is a key component. Among many semiconductor photocatalysts, g-C3N4 has attracted great attention due to its narrow band gap, excellent stability and low cost. However, practical application is limited by its poor intrinsic activity. In this work, a high-performance porous g-C3N4 (PCN) photocatalyst with anchored Cu single atoms (CuSAs) was synthesized by a one-step co-heating approach. The obtained Cu1.5–PCN displays an excellent hydrogen evolution rate (HER) of 2142.4 μmol h−1 g−1 under visible light (=420 nm), which is around 15 and 109 times higher than those of PCN and bulk g-C3N4, respectively. In addition, it also shows good stability during H2 evolution. The results of experimental research and DFT simulations indicate that the single Cu ions formed bonds with the N-ring and these remain stable. Meanwhile, the special electronic structure of the Cu–N charge bridge extends the light absorption band to the visible-light region (380–700 nm). This high-performance and low-cost photocatalyst has great potential in solar energy conversion.
研究领域:
材料科学
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能源化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Ziheng Zhen,Antai Li,Tiantian Xiao,Maoshuai Li,Jing Lv,Shouying Huang,Yue Wang,Xinbin Ma
Bimetallic catalyst with dual-atom pairs has drawn much attention in heterogeneous catalysis due to their unique synergistic effects. In this work, we prepared a series CeO 2 supported Cu-Pt dual sites catalysts and found the optimized one of 2Cu0.025Pt/CeO 2 exhibited excellent performance in the hydrogenation of methyl acetate (MA). Its product yield of ethanol was as 4 times as that of 2Cu/CeO 2 catalyst under the same reaction conditions, with only 0.025 wt% Pt addition. Combined with various characterizations and contrast samples, it is demonstrated that the post-deposited trace Pt species preferentially located besides the copper atoms and formed Cu-Pt atomic pairs. But when further increasing the loading of Pt, the aggregation of Cu happened, leading to a rapid decrease of activity. To reveal the role of Cu-Pt atom pairs in the hydrogenation of carbon–oxygen bonds reactions, we conducted chemisorption experiments and DFT simulations. It is suggested that Cu-Pt atomic pairs significantly enhanced the adsorption and activation capability of both the MA and H 2 molecules during the reaction. These insights may provide synthesis and design strategy for high-performance dual-atom sites catalysts for the carbon–oxygen bonds hydrogenation reactions.
研究领域:
催化化学
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材料科学
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理论计算
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产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Jian Li,Shuai-Bing Ma,De-Sheng Wei,Wan-Yi Lan,Ting-Ting Xu,Yu-Teng Zhang,Nan Lv,Shuang-Bao Li
Herein, a novel CF 3 -functionalized zirconium-based metal-organic tetrahedron (ZrT-(CF 3 ) 2 ) was constructed based on 2.5-bis(trifluoromethyl)terephthalic acid (H 2 BDC-(CF 3 ) 2 ) ligand and trinuclear zirconocene building unit. Notably, the single crystals of ZrT-(CF 3 ) 2 was obtained under traditional solvothermal condition, while the yield and purity could be further improved by the microwave-assisted solvothermal method. Subsequently, the adsorption performance of ZrT-(CF 3 ) 2 for salicylic acid (SA) emerging contaminant was systematically evaluated, indicating a maximum adsorption capacity of 99.91 mg/g under optimal conditions. Furthermore, a possible adsorption mechanism was proposed based on experimental results and DFT simulations.
研究领域:
材料科学
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环境科学
·
化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Qianqian Ni,Huiping Shao,Yun Zhang,Xin Ke,Wengang Liu
Oxygen vacancies could be induced into the heterojunction structure of BiOI/BiOBr via high-temperature calcination. Light absorption, charge transfer efficiency, photocatalytic activity, and mechanism are all intimately connected to oxygen vacancies. Density-functional theory simulations demonstrate that surface oxygen vacancies adsorb oxygen to active sites, whereas bulk oxygen vacancies activate oxygen adsorbed to the surface to reactive radicals. Meanwhile, the addition of oxygen vacancies efficiently reduces the effects of background ions and pH on tetracycline breakdown in the real aquatic environment. The experimental results are consistent with the DFT calculations. This paper presents a straightforward approach for creating heterojunction surface and bulk-phase oxygen vacancies, as well as an understanding of the many roles that different types of oxygen vacancies play in the photocatalytic degradation process.
研究领域:
环境科学
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材料科学
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光催化化学
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水污染治理
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计算化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yangbo Ma,Miao Fa,Yihui Zhang,Liuying Xiong,Xiying Li,Shuaishuai Zhou,Wei Chen,Liqun Mao
Precious metals loading strategy is an effective method to increase the reactivity of CdS based photocatalysts for hydrogen evolution from water splitting under visible light. The key problem of such strategy is the affecting mechanism, which determined by the composition, species and structure of the loaded metals. In this study, AgPd bimetallic nanoclusters (Ag x Pd y ) were prepared and then loaded onto the surface of snowflake-like CdS and the affecting mechanism was qualitatively and quantatively investigated through both instrumental analysis and computational method. The composition and structure of synthesized samples were examined through XRD, TEM, and XPS, by which the successful synthesis of AgPd bimetallic nanocluster alloys with an average particle size of approximately 3 nm were confirmed. Further, the hydrogen evolution performance of Ag x Pd y /CdS was tested under visible light and the prepared AgPd 3 /CdS achieved a hydrogen evolution rate of 73.93 mmol h −1 g −1 , which is a 28 % improvement over Pd/CdS and a 381 % improvement over CdS, with an AQY of 44.68 % at 420 nm. The photoelectrochemical tests (LSV, I-T, EIS, PL, and TR-PL), ESR, and TRPL were applied to qualitatively demonstrate the function of Ag x Pd y nano-cocatalyst, and the testing results indicated that the cocatalyst significantly enhances the separation and transfer efficiency of photoinduced electrons, while further lowering the hydrogen evolution reaction energy barrier. Based on that, affecting mechanism was further determined through DFT simulation quantitatively. The prediction results indicated that the unique nanoclusters structure of AgPd 3 contribute with the high work function and low d band center position increase the transfer efficiency of the photoinduced charge carriers. This study quantitatively revealed the relationship among compostion, structure and reactivity of the photocatalysts, provided an method to investigate the affecting mechanism of bimetallic hydrogen evolution photocatalysts and contributed to the advancement of renewable energy development.
研究领域:
材料科学
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可再生能源
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催化化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 41
·94740-94756
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IF 5.8
Zhao Xiaoben,Chen Guanyu,He Song,Sheng Hongliang,Sun Junwei,Wu Xiya,Tian Fuliang,Zhang Xiaoqian
The cyclohexane is the common toxic volatiles emitted from the various industry in worldwide leading to environmental degradation and human illnesses. Hence, there is a requirement for an efficient and stable adsorbent for adsorbing these toxic molecules to safeguard human health and the air atmosphere. Hollow carbon spheres (HCS) are a new type of carbon nanomaterial with large specific surface area, low density, and good chemical and thermal stability. In this study, DFT simulations and static-dynamic adsorption studies of cyclohexane were carried out using HCS as the adsorbent material. Among them, static adsorption focuses on adsorption/desorption isotherm, adsorption isotherm model fitting and isosteric heat of adsorption. Dynamic adsorption was mainly studied the effect of initial concentrations, gas flow rate, and ambient temperature on adsorption performance. The results showed that HCS exhibited very good performance in cyclohexane adsorption.
研究领域:
环境科学
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材料科学
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化学工程
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计算化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jiayi Shan,Fei Ying,Linrui Li,Yubo Pan,Ziwen Shi,Jijia Liang,Yunfei Gao,Fengyun Wang,Mingzhu Xia
The development of high-efficiency adsorbents for addressing Pb(II) contamination in aquatic environments remains an urgent challenge in environmental remediation. This study presents a novel thiol-functionalized ZIF-8-based adsorbent (ZIF-8-TMT) with a stable 3D framework and abundant thiol groups, designed to overcome the limitations of conventional adsorption materials. The synthesized ZIF-8-TMT demonstrated a substantial BET surface area (456.58 m 2 /g) and numerous active adsorption sites, exhibiting exceptional Pb(II) adsorption capacity (494.9 mg/g) that surpassed most previously reported adsorbents. Systematic characterization revealed that the composite achieved rapid adsorption kinetics, with approximately 80 % removal efficiency within 30 min, and maintained excellent regenerability - showing negligible capacity reduction after three adsorption-desorption cycles and retaining over 60 % removal efficiency after five cycles. The adsorption mechanism was comprehensively investigated through Fourier-transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and computational simulations including density functional theory (DFT), bond order density (BOD), and natural adaptive orbital (NAdO) analyses. Results indicated that the superior adsorption performance originated from synergistic effects between electrostatic interactions and dual coordination involving the N3 atoms in 2-methylimidazole ligands and thiol (-SH) groups from TMT. This study not only provides fundamental insights into the coordination chemistry of Pb(II) adsorption but also demonstrates the practical potential of ZIF-8-TMT for wastewater treatment applications, offering a promising solution for heavy metal pollution control with its combination of high capacity, rapid kinetics, and excellent reusability.
研究领域:
环境科学
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材料化学
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重金属修复
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吸附技术
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 13
·4741-4752
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IF 10.182
Song Li,Qiaozhi Ma,Wenxin Zhong,Xuelai Zhao,Xiangqian Wei,Xinghua Zhang,Qiying Liu,Chenguang Wang,Longlong Ma,Qi Zhang
Catalytic hydrodeoxygenation of bioderived furans is critically attractive to prepare sustainable fuels. Herein, a novel octanediol-route was developed to produce octane through one-pot conversion of bioderived furans at low temperatures. A 96.6% yield of octane was obtained by catalytic conversion with Pd/C and phosphotungstic acid (HPW). Experimental validation of the novel pathway revealed that octanediol intermediates could be formed through hydrogenolysis of furans before deoxygenation. The spontaneous process of this octanediol-route was thermodynamically confirmed by DFT simulations. In addition, characterization studies suggested that water in the system strengthened the cooperation between metals and acids to facilitate C–O bond scission through the modification and hydrogen transfer of HPW. This work highlights a promising reaction pathway for an efficient HDO catalytic system to obtain alkanes from bioderived furans under mild conditions.
研究领域:
催化
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可持续化学
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可再生能源
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产品关联
DOI
高影响因子
MINERALS ENGINEERING
·
2022
·
IF 5.479
Haiping Zhao,Xiaopeng Niu,Bingxu Dong,Xianbing Jia,Renman Ruan
This work aims to establish the quantitative relationship between the surface oxidation state of pyrite and flotation performance. In this paper, an efficient method was proposed to prepare pyrite with different oxidation degrees. Flotation tests show that the floatability of pyrite decreased with prolonging the oxidation time. Tof-SIMS results reveal that the main component on the oxidized pyrite surface is Fe hydroxides or oxides. XPS analysis confirms that Fe(OH) 2 and FeOOH are the main formula of Fe species, and the ratio of Fe 2+ /Total Fe agrees well with the floatability of pyrite with different oxidation degrees, which can be taken as an index to develop the flotation performance of pyrite. DFT simulation calculation further demonstrates the reliability of Fe(OH) 2 as the active site. This study provides essential surface chemistry evidence for correlating the surface species with the floatability of pyrite with different oxidation states through quantitative analysis of various intermediate products.
研究领域:
矿物加工
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表面化学
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材料科学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Rongchuang Geng,Hanxiao Tang,Qiujuan Ma,Luping Liu,Weisheng Feng,Zhijuan Zhang
In this work, a series of bimetallic Ag/Zn-ZIF-8 materials were successfully developed for sensing toward traces of Fe 3+ and Cu 2+ . The bimetallic Ag/Zn-ZIF-8 was synthesized via a one-pot method. Interestingly, this obtained bimetal Ag/Zn-ZIF-8 exhibited high photoluminescence property and excellent fluorescence quenching response to target analytes with high selectivity , sensitivity and detection limits of 3.9 μM for Fe 3+ , 6.7 μM for Cu 2+ ions, respectively, both of which have been confirmed to be very comparable or better than the reported LMOFs sensors. The possible photoluminescence quenching mechanisms were studied in detail, revealing that the competitive absorption of excitation source and resonance energy transfer (RET) resulted from the host (imidazole of the framework, Lewis basic sites)-guest (metal ions of Cu 2+ and Fe 3+ , Lewis acid sites) interaction should be responsible for high efficiency fluorescence quenching. The binding energies of metal ions adsorption on the ZIF-8 obtained by DFT simulation were further performed to explain the higher quenching effect of Fe 3+ than Cu 2+ .
研究领域:
材料科学
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分析化学
·
纳米技术
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Dexiang Zhang,Fujun Lan,Xiaomei Zhou,Yu Shu,Fu Li,Qingxin Guan,Mo Qiu,Wei Li
Amino acids are widely used in various applications, its production mainly relies on the fermentation of grain crops, and the chemosynthesis method from non-grain biomass still faces the challenge of low efficiency (<50 %). Herein, Ru clusters anchored on ultrathin TiO 2 nanobelts (NBs) with abundant oxygen vacancies are fabricated and used to convert lignocellulose-derived α-hydroxy acids to α-amino acids. The Ru/TiO 2 NBs achieved up to 80 % alanine yield from lignocellulose-derived lactic acid (LA). The characterization results reveal that the TiO 2 NBs with abundant oxygen vacancies could anchor Ru clusters uniformly and enable the α-OH dehydrogenation occur spontaneously. Simultaneously, Ru clusters with appropriate particle size are beneficial for the activation of H 2 and could promote the dehydrogenation from the α-OH and α-C(sp 3 )-H of LA. Furthermore, DFT simulations also indicate that further decrease the Ru cluster size (< 1 nm) will inhibit the adsorption of α-C(sp 3 )-H on cluster surface, thereby suppressing the removal of hydrogen atoms. This research provides a green and efficient chemical catalytic conversion idea for amino acid production from non-grain biomass.
研究领域:
催化
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纳米材料
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绿色化学
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生物质转化
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Haimeng Huang,Jianfeng Zhang,Chunmei Tang,Anyu Li,Tianmeng Zhang,Huapeng Xue,Daofeng Zhang
Photocatalytic sterilization has been recently realized as a competitive strategy for effective water purification just using sunlight, for which the new photocatalytic materials play the key role. In this study, a novel Z-scheme heterojunction material MXene/TiO 2 /Bi 2 S 3 was proposed, where TiO 2 nanoparticles and Bi 2 S 3 microspheres were uniformly distributed on the MXene nanosheets through facile hydrothermal oxidation and ultrasonic dispersion. With this Z-scheme heterojunction MXene/TiO 2 /Bi 2 S 3 , effective and quick sterilization of both Gram-negative bacteria and positive bacteria in only 120 min was realized. Especially, the apparent reaction constant for S. aureus reached 0.01659 min −1 , substantially higher than MXene and other related materials in literature. This could be ascribed to the narrow band gap (1.04 eV), the wide range of light absorption range (420 nm), and the low impedance of the as-obtained composite, facilitating the transfer and separation of photo-generated charges, which was also validated through the first-order kinetic model and DFT simulation calculations. Thus, the reactive species produced by photocatalysis effectively disrupted the defense action of the bacteria by damaging bacterial membrane structure, and reducing enzyme activity as well as cellular metabolism. This efficient and low-cost material for water disinfection has a great potential for practical applications in the future.
研究领域:
环境科学
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材料科学
·
化学
✓ 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）