ACS Catalysis
·
2025
·
IF 13.1
Luyao Ge,Heng Liang,Wei Lan,Maodi Wang,Xiaoming Zhang,Aiping Jia,Xiang-Kui Gu,Qihua Yang,Xiaobo Li
Enzyme cofactor-mediated biochemical cascades in living cells showcase nature’s capacity for efficient, selective multistep transformations, inspiring artificial chemoenzymatic systems that merge enzymatic specificity with the versatility of synthetic catalysts via the cofactor. Practical implementation of such systems is, however, constrained by poor selectivity, enzyme incompatibility, and limited turnover in nonenzymatic in situ cofactor regeneration. Here, molecular ligand-directed interfacial tailoring of supported Pt catalysts is shown to overcome these challenges, achieving >99% regioselective NADH regeneration from NAD+ with H2 as a clean reductant, while enhancing the activity and stability. Machine learning-guided analysis of a structurally diverse ligand library, validated experimentally, identifies the surface Pt2+ fraction as a robust, predictive electronic descriptor for selectivity classification across catalyst variants. Integration of the ligand-optimized catalyst with an NADH-dependent dehydrogenase delivers asymmetric hydrogenations with >99% enantiomeric excess and benchmark in situ NADH turnover numbers. This study demonstrates an H2-driven chemoenzymatic platform that bridges heterogeneous metal catalysis and enzymatic catalysis, offering immediate relevance to a wide range of applications, including fine chemical synthesis and artificial photosynthesis.
研究领域:
催化化学
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合成生物学
·
化学工程
·
生物催化
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化学中的机器学习
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可持续化学
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产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2020
·Vol. 22
·期 7
·3953-3958
·
IF 3.43
Jingbo Qi,Xun Hu
The reduction of ZnO in a ZnO-supported catalyst to metallic zinc, the alloying of metallic zinc with a second metal and the evaporation of zinc species in a reductive atmosphere of hydrogen was investigated in this study. The results show that the reduction temperature was the determining factor for the transformation of zinc species. The complete removal of ZnO in a ZnO-supported catalyst can be achieved at 700 °C. The effects of different metals supported on ZnO on the transformation of ZnO were also investigated. Cu, Co and Ni species can slow the ZnO loss due to the priority for the reduction of these metal oxides and the formation of metal–Zn intermetallics. Fe based catalysts noticeably accelerated the loss of ZnO, which can be ascribed to the high oxophilicity of Fe and the strong interactions between the metal and support.
研究领域:
化学工程
·
催化科学
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DOI
高影响因子
Scientific Reports
·
2017
·Vol. 7
·期 1
·1-11
·
IF 4.259
Zhao Jiangtao,Zhang Peng,Wang Zhuo,Zhang Shijie,Gao Hongqing,Hu Junhua,Shao Guosheng
In the field of photocatalysis, the high-charge recombination rate has been the big challenge to photocatalytic conversion efficiency. Here we demonstrate the direct evidence of multichannel-improved charge-carrier mechanism to facilitate electron-hole transfer for raising photocatalytic H 2 evolution activity. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and UV-Vis diffuse reflectance spectroscopy (DRS), were used to characterize the as-fabricated samples. The result shows that the present design of Au/Pt nanoparticles (NPs) decorated one-dimensional Z-scheme TiO 2 /WO 3 heterostructure composite nanofibers have been fabricated, which even exhibited excellent light absorption in the visible region and greatly enhanced photocatalytic activities on H 2 generation comparing with pure TiO 2 , TiO 2 /WO 3 and Pt/WO 3 /TiO 2 nanofibers. This greatpromotion is mainly on account of the photosynthetic heterojunction system, which include the surface plasmon resonance (SPR) of Au nanoparticles, low overpotential of Pt nanoparticles, and more importantly, the one-dimensional multichannel-improved charge-carrier photosynthetic heterojunction system with Pt as an electron collector and WO 3 as a hole collector. Transferring photoinduced electrons and holes at the same time, leading to effective charge separation was directly proved by ultraviolet photoelectron spectroscopy, electrochemical impedance spectroscopy, photocurrent analysis and incident photon-to-electron conversion spectrum.
研究领域:
材料科学
·
能源化学
·
环境科学
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DOI
高影响因子
Advanced Science
·
2026
·
IF 14.1
Jinju Cai,Mengping He,Jianya Luo,Shuang Zhou,Tengyue Zhang,Jianing Li,Zhiqiang Wang,Yuan Liu
Plasmid-mediated colistin resistance gene mcr has markedly diminished the effectiveness of colistin in managing multidrug-resistant (MDR) Gram-negative bacterial infections. Employing antibiotic adjuvants to revive colistin susceptibility offers a valuable solution to address this issue. Intestinal pathogens have evolved sophisticated acid resistance systems to withstand the acidic environment, a key adaptation that facilitates subsequent infection. Utilizing transposon sequencing, here we identify yqgB gene as a crucial target for restoring colistin susceptibility in mcr -positive bacteria, particularly under acidic conditions. yqgB deficiency drastically enhances colistin's bactericidal effect, which is attributed to the alteration of phospholipid composition and reduction in lipopolysaccharide modification. Using deep learning-based screening, we find that H 2 receptor antagonists (ebrotidine, ranitidine and famotidine) can act as dual inhibitors of MCR and YqgB proteins, thus exhibiting excellent synergistic activity with colistin against mcr -positive bacteria under both neutral and acidic conditions. This combination not only bolsters colistin's efficacy but also impedes the evolution and spread of colistin resistance. In animal models infected with mcr -positive pathogens, the co-administration of ranitidine and colistin demonstrates superior therapeutic outcomes against both systemic and intestinal infections. Our findings highlight the potential of targeting the bacterial acid stress response system to counteract mcr -mediated colistin resistance and offer a promising therapeutic strategy for the treatment of MDR bacterial infections.
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DOI
PubMed
高影响因子
AICHE JOURNAL
·
2026
·
IF 4
Puxin Shi,Liping Luan,Bo Zhang,Islam Mohammad Mahfuzul,Zhi Wang,Xinlei Liu
High-performance H 2 /CO 2 separation with good scalability is needed in industry. Here, we fabricated mixed polymer fragment membranes on alumina tubes. The synergistic control of monomer diffusion rate promoted the formation of H 2 selective channels, thereby elevating the H 2 /CO 2 separation performance. The membranes, each with an area of 37.7 cm 2 , demonstrated a high H 2 /CO 2 selectivity of 22.5 (with a corresponding H 2 permeance of 209 GPU) at 150°C and 2 bar, high pressure resistance (H 2 permeance and H 2 /CO 2 selectivity were 212 GPU and 11.1 at 200°C and 10 bar, respectively), and good reproducibility. Furthermore, we studied the effects of sweep gas, permeate pressure, reuse of substrates, and H 2 O and H 2 S contaminants on membrane performance, pointing out that the membranes can be well adapted to industrial relevant conditions. In addition, a two-stage membrane system was designed to produce high concentration H 2 with a good yield.
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产品关联
DOI
高影响因子
iScience
·
2021
·
IF 5.458
Anhui Zheng,Yuxuan Wang,Fangfei Zhang,Chunnian He,Shan Zhu,Naiqin Zhao
To achieve net-zero emissions, a particular interest has been raised in the electrochemical evolution of H 2 by using catalysts. Considering the complexity of designing catalyst, we demonstrate a data-driven strategy to develop optimized catalysts for H 2 evolution. This work starts by collecting data of Pt/carbon catalysts, and applying machine learning to reveal the importance of ranking various features. The algorithms reveal that the Pt content and Pt size have the greatest impact on the catalyst overpotentials. Following the data-driven analysis, a space-confined method is used to fabricate the size-controllable Pt nanoclusters that anchor on nitrogen-doped (N-doped) mesoporous carbon nanosheet network. The obtained catalysts use less platinum and exhibit better catalytic activity than current commercial catalysts in alkaline electrolytes. Moreover, the data formed in this work can be used as feedback to further improve the data-driven model, thereby accelerating the development of high-performance catalysts.
研究领域:
电化学
·
材料科学
·
人工智能
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Qi Li,Pengcheng Wu,Yufan Huang,Peng Chen,Keliang Wu,Jianning Wu,Yan Luo,Lele Wang,Shengchao Yang,Zhiyong Liu,Xuhong Guo
Traditional surface-to-surface contact heterojunctions suffer from poor stability and low electron-hole separation efficiency, which has become a crucial limiting the further improvement of photocatalytic property. Therefore, improving the combination of heterogeneous materials will become a new attempt. In this work, a novel lattice embedded ZnO@TiO 2 (B) nanoflowers was prepared by combining electrodeposition method combined with hot solvent method. The hetero interface of the ZnO@TiO 2 (B) nanoflowers is distributed in the phase of TiO 2 (B), which drives high-efficiency charge separation. The sample Zn:Ti 1:4 has the highest photocatalytic property, and the H 2 generation efficiency under the full spectrum is 1.695 mmol g −1 h −1 , which is 3.5 times that of TiO 2 (B). After 36 h cycle stability test, its stability is as high as 90%. According to results, the possible mechanism of ZnO@TiO 2 (B) photocatalytic hydrogen production is proposed. These findings may provide new strategies for the preparation of high-efficiency heterojunction photocatalysts with special structures.
研究领域:
材料科学
·
光催化
·
纳米材料
·
能源化学
·
半导体物理
·
环境功能材料
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DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2020
·Vol. 34
·期 9
·e5745
·
IF 3.14
Yong-Lai Liu,Zhen-Xiang Dai,Zi-Feng Yao,Gan-Hong Zheng,Yong-Qing Ma
SrMoO 4 and Mn-doped SrMoO 4 nanoparticles have been synthesized by high temperature thermal decomposition of metal–organic salt in organic solvent with a high boiling point. Then they were reduced in H 2 /N 2 mixture atmospheres at different reducing temperatures T R . Samples were characterized by X-ray diffraction (XRD), UV–visible light spectrum (UV), and X-ray photoelectron spectroscopy (XPS). The XRD and XPS results showed that SrMoO 3 phase appears when the annealing temperature was 700 °C (SMO700). The light absorption edge shifted to the visible range and enhanced the visible light photocatalytic activity. The methyl blue (MB) solution was degraded, and the degradation efficiency was 80.30% in 120 min for SMO700 sample. For the 2%Mn doping SrMoO 4 sample, the efficiency of degradation reached 97.53% when the annealing temperature was 700 °C(2Mn-SMO700). The results showed that a certain amount of SrMoO 3 is helpful to improve the photocatalytic performance of SrMoO 4 . In addition, the photocatalytic performance of SrMoO 4 was also related to Mn-doped amount, annealing temperature and annealing time in H 2 /N 2 mixture atmospheres. The related mechanism was discussed.
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DOI
高影响因子
ChemCatChem
·
2019
·Vol. 11
·期 24
·6391-6397
·
IF 4.495
Huifan Li,Gaifang Pan,Mengna Ding,Wenkai Pei,Ziping Zhang,Yingchun Miao,Yuning Huo
Ag/Bi 2 WO 6 microspheres were successfully prepared by ultrasound-assisted photo-reduction route to realize the Ag-loading on Bi 2 WO 6 crystal, which was previously synthesized by using solvothermal process with [C 4 -mim]BF 4 ionic liquid. The synergistic process of photo-reduction and ultrasonic irradiation induced the efficient conversion of Ag + ion into metallic Ag nanoparticles with uniform distribution. The enhanced amount of Ag nanoparticles and the strong combination of Ag nanoparticles with Bi 2 WO 6 microspheres, efficiently promoted the light harvesting and inhibited the recombination of photo-induced charges. As a result, Ag/Bi 2 WO 6 microspheres via ultrasound-assisted photo-reduction route achieved the higher visible-light photocatalytic activity for H 2 evolution than those catalysts prepared by other methods. This work may provide an efficient way for designing photocatalysts for hydrogen generation using solar light. Graphical Photocatalysis : The synergistic process of photo-reduction and ultrasound irradiation was utilized to achieve the uniform Ag-loading on Bi 2 WO 6 microspheres. The enhanced amount of Ag nanoparticles and their strong combination with Bi 2 WO 6 crystals was beneficial for improving visible-light absorption, and inhibiting recombination of photo-generated charges. It resulted in the promoted activity for visible-light photocatalytic H 2 evolution.
研究领域:
材料科学
·
光催化
·
纳米技术
·
氢能
·
环境科学
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DOI
高影响因子
POLYHEDRON
·
2021
·
IF 3.052
Aihong Li,Dongyang Li,Jianwei Mao,Zhimeng Ge,Jianping Guo,Bo Liu
Through a facile solvothermal method, the novel composites of cobalt(II) diphenylphosphinate/TiO 2 have been synthesized and used for photocatalytic hydrogen production in ethanol solution. The chemical composition and surface morphology were analyzed by XPS, XRD, ICP-OES, EA, IR and SEM. The composite CoTi10 showed high photocatalytic activity in H 2 evolution that the quantity is ca. 1155.86 μmol/g for 3 h in ethanol solution under the illumination of UV–visible light source, which is 12 times higher than the commercial P25. The composites also exhibited unique selectivity for converting ethanol to 1,1-diethoxyethane in the photocatalytic process. Moreover, their good stabilities were revealed in the recycling test. It is thus clear that the composite can effectively inhibit the recombination of electron-hole pairs in photocatalytic reactions and lead to the enhanced hydrogen production rate.
研究领域:
材料科学
·
光催化
·
氢能
·
化学工程
·
可持续能源
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 54
·期 6
·4811-4820
·
IF 2.993
Qin Hengfei,Lv Wenhua,Bai Jirong,Zhou Yue,Wen Yingpin,He Qinting,Tang Jianghong,Wang Liangbiao,Zhou Quanfa
Graphitic carbon nitride (g-C 3 N 4 ) is considered as an attractive, efficient and newly generated photocatalyst material owing to its distinct properties such as metal free, suitable band gap and high physicochemical stability. Nevertheless, the photocatalytic activity of pure g-C 3 N 4 was limited by the fast recombination rate of photoinduced electron–hole pairs and relatively low specific surface area. In this study, we provide a new prospect to overcome the problem by using another suitable precursor urea-assisted copolymerization with thiourea which is expected to optimize the process of thermal condensation, inhibit agglomeration and improve the specific surface area; meanwhile, the formed isotype heterogeneous junction effectively inhibits charge carrier recombination. The formed g-C 3 N 4 isotype heterojunction photocatalyst manifested significant improvement photocatalytic hydrogen production than the single and pure g-C 3 N 4 sample. This significant enhanced photocatalytic performance is mainly ascribed to inhibited recombination, enriched active site and enlarged specific surface area.
研究领域:
材料科学
·
光催化
·
氢能
·
纳米材料
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DOI
高影响因子
ACS ES&T Engineering
·
2024
·
IF 7.4
Yanke Yu,Jiahang Li,Mengqiao Geng,Yonghua Zhao,Reem Albilali,Chi He
Catalytic oxidation of industrial aromatic hydrocarbons at low temperatures is still a challenge. In this work, we found that H2 can significantly promote toluene oxidation over Pt/TiO2 catalyst by intrinsically altering the reaction route, with the temperature at conversion of 90% (T90) decreasing from 199 to 146 °C and apparent activation energy reducing from 109.2 to 38.6 kJ·mol−1. Moreover, CO2 selectivity increases to 100% at 180 °C, which is much higher than that without H2 (just 30.2%). H2 also benefits maintenance of Pt0 in the reaction and thus promotes catalyst stability. Based on the results of temperature-programmed surface reaction, in situ DRIFTS, in situ Raman, and theoretical calculations, the toluene oxidation mechanism over Pt/TiO2 changes greatly after the addition of H2. Without H2, −CH3 of toluene is oxidized first, and the reaction pathway follows a traditional way of toluene → benzyl alcohol → benzaldehyde → benzoic acid → maleic acid → CO2 and H2O. However, the C−C bond of toluene is broken first in the presence of H2, and benzene is formed by the hydrodealkylation process. The reaction mainly follows the pathway of toluene → benzene → phenol → benzoquinone → maleic acid → CO2 and H2O. In addition, H2 also significantly promotes the oxidation of p-, m-, o-xylene, and ethylbenzene. This work sheds a new viewpoint to realize the low-temperature and eco-friendly purification of toluene and benefits the development of efficacious catalytic systems toward volatile organic compound degradation.
研究领域:
催化化学
·
环境化学
·
材料科学
·
化学工程
·
物理化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）