INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
·
IF 8.3
Weijing Cao,Xu Chen,Fulong Liu,Xiaoli Gu,Yan Qing,Zupeng Chen
Lignocellulose biomass, a plentiful and renewable resource found in abundance on Earth, holds significant promise in reforming into H 2 and value-added biochemicals like lactic acid through photocatalytic technology. However, the efficient photorefinery encounters challenges, including the recombination of photo-induced carriers, poor H 2 evolution, and slow biomass oxidation. Here, we report a bimetallic catalyst supported on layered carbon nitride (PtRh/CN) for lignocellulose photoreforming. This catalyst combines the synergistic effects of Pt and Rh, enhancing both the absorption of visible light and the separation and migration of photogenerated charge carriers. The optimal catalyst achieves a high hydrogen production rate of 6.1 mmol g −1 h −1 and a lactic acid yield of 92.9 %. Mechanistic studies using specific scavengers demonstrate that e − , h + , 1 O 2 , ⋅O 2 − , and ⋅OH species all facilitate the simultaneous production of hydrogen and lactic acid. This study not only advances the efficient utilization of lignocellulose biomass but also provides a novel framework for designing highly efficient photocatalysts for photoreforming biomass into hydrogen and biochemicals.
研究领域:
光催化
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生物质转化
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能源化学
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环境科学
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材料科学
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可再生能源
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绿色化学
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高影响因子
Catalysts
·
2025
·Vol. 15
·期 3
·212
·
IF 4
Yu Wang,Xuemin Cao,Yuting Dai,Tao Yan,Xiangjie Zhang,Huizi He,Yujie Xie,Tiejun Lin,Chang Song,Peng He
This study investigates the hydroformylation of C5+olefins derived from Fischer–Tropsch synthesis (FTS) using Rh-based catalysts supported on zeolites (MFI, MEL) and SiO2. A series of catalysts were synthesized through two different methods: a one-pot hydrothermal crystallization process, which results in highly dispersed Rh species encapsulated within the zeolite framework (Rh@MFI, Rh@MEL), and an impregnation method that produces larger Rh nanoparticles exposed on the support surface (Rh/MFI, Rh/MEL, Rh/SiO2). Characterization techniques such as BET, TEM, and FTIR were employed to evaluate different catalysts, revealing significant differences in the dispersion and accessibility of Rh species. Owing to its more accessible mesoporous structure, Rh/SiO2with a pore size of 5.6 nm exhibited the highest olefin conversion rate (>90%) and 40% selectivity to C6+aldehydes. In contrast, zeolite-encapsulated catalysts exhibited higher selectivity for C6+aldehydes (~50%) due to better confinement and linear aldehyde formation. This study also examined the influence of FTS byproducts, including paraffins and short-chain olefins, on the hydroformylation reaction. Results showed that long-chain paraffins had a negligible effect on olefin conversion, while the presence of short-chain olefins, such as propene, reduced both olefin conversion and aldehyde selectivity due to competitive adsorption. This work highlights the critical role of catalyst design, olefin diffusion, and feedstock composition in optimizing hydroformylation performance, offering insights for improving the efficiency of syngas-to-olefins and aldehydes processes.
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BIORESOURCE TECHNOLOGY
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2016
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IF 4.917
Jing Yang,Liang Zhao,Chunze Liu,Yuanyuan Wang,Liyi Dai
Efficient catalytic ethanolysis and gasification of kraft lignin were conducted over a versatile supported catalyst Rh/La 2 O 3 /CeO 2 –ZrO 2 to give high-value aromatic alcohols and H 2 -rich gas. The removal of phenolic hydroxyl group was the most prevalent reaction, and importantly, almost no phenols, undesired char and saturating the aromatic ring were detected. Meanwhile, the feedstock and solvent both played key roles in H 2 generation that contributed to the hydrodeoxygenation of liquid components and made the whole catalytic process out of H 2 supply. Reusability tests of catalyst indicated that the crystalline phase transition and agglomeration of support, the loss of noble metal Rh and carbon deposition were the possible reasons for its deactivation in supercritical ethanol. Comparing with water, methanol and isopropanol system, ethanol was the only effective solvent for the depolymerization process.
研究领域:
化学工程
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能源科学
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高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
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2021
·Vol. 19
·期 1
·1-21
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IF 10.435
Wang Tian-Long,Zhou Zi-Fei,Liu Jun-Feng,Hou Xiao-Dong,Zhou Zhi,Dai Yun-Lu,Hou Zhi-Yong,Chen Feng,Zheng Long-Po
Background Skin injury and the resultant defects are common clinical problems, and usually lead to chronic skin ulcers and even life-threatening diseases. Copper, an essential trace element of human body, has been reported to promote the regeneration of skin by stimulating proliferation of endothelial cell and enhance angiogenesis. Results Herein, we have prepared a new donut-like metal–organic frameworks (MOF) of copper-nicotinic acid (CuNA) by a simple solvothermal reaction. The rough surface of CuNA is beneficial for loading/release basic fibroblast growth factor (bFGF). The CuNAs with/without bFGF are easily processed into a light-responsive composite hydrogel with GelMA, which not only show excellent mechanical properties, but also display superior biocompatibility, antibacterial ability and bioactivity. Moreover, in the in vivo full-thickness defect model of skin wound, the resultant CuNA-bFGF@GelMA hydrogels significantly accelerate the wound healing, by simultaneously inhibiting the inflammatory response, promoting the new blood vessels formation and the deposition of collagen and elastic fibers. Conclusions Considering the superior biocompatibility, antibacterial ability and bioactivity, the CuNA and its composite light-responsive hydrogel system will be promising in the applications of skin and even other tissue regeneration. Graphic abstract
研究领域:
材料科学
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生物材料
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组织工程
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生物医学工程
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药剂学
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DOI
PubMed
高影响因子
Materials Today Bio
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2026
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IF 11
Bangxun Mao,Binge Huang,Mengru Li,Wentao Zhang,Qian Chang,Xiaojun He,Shihao Xu
The rising incidence of multidrug-resistant (MDR) bacterial infections in deep tissues, such as subcutaneous abscesses and bacterial pneumonia, has become an urgent public health concern. Both conventional antibiotic treatments and nanomaterial-based therapies are inadequate due to their limited catalytic efficiency, poor tissue penetration, and the enhanced resistance they provoke. We report the rational design and synthesis of nitrogen-doped rhodium single-atom catalysts (Rh SACs) that integrate second near-infrared (NIR-II) photothermal conversion with multienzyme mimetic activities. This nanozyme platform employs a synergistic ‘photothermal-catalytic’ therapy to effectively eliminate MDR pathogens and disrupt biofilms. Density functional theory (DFT) calculations indicate that atomically dispersed Rh sites lower the reaction barrier and optimize the adsorption of intermediates. The presence of rhodium enhances peroxidase and oxidase-mimetic activities under NIR-II irradiation. Transcriptional analysis reveals that Rh SACs modulate inflammation signaling and the immune microenvironment at the molecular level. In mice with methicillin-resistant Staphylococcus aureus -infected abscesses and lung infections, treatment with Rh SACs resulted in nearly complete bacterial clearance, biofilm disruption, and accelerated tissue repair. Additionally, macrophage polarization shifted significantly from M1 to M2. A systematic biosafety assessment demonstrated excellent hemocompatibility and minimal systemic toxicity. This work not only presents an efficient and resistance-free strategy for treating deep tissue infections but also provides crucial structural insights for structure-activity relationship studies in single-atom nanozymes. We strongly believe that nanosystems hold substantial potential for clinical translation in catalytic nanomedicine.
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PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 19
·5686-5693
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IF 7
Hongjing Wang,Yuqin Liang,Songliang Liu,Xu Mu,Hongjie Yu,Kai Deng,Ziqiang Wang,You Xu,Liang Wang
Coupling the thermodynamically favorable sulfion oxidation reaction (SOR) with the hydrogen evolution reaction (HER) is a promising approach to simultaneously save energy and cost-effectively produce high value-added chemicals and hydrogen. The construction of efficient bifunctional catalysts for SOR–HER electrocatalysis is of significance yet challenging. Here, we propose a dual-nonmetal-doping strategy to construct S and P dual-doped Rh metallene (SP-Rhlene). Benefiting from the combined advantages of dual heteroatom doping and an ultrathin nanosheet structure, SP-Rhlene with a large electrochemical active area and an optimized electronic structure exhibits outstanding HER and SOR activities. A two-electrode system based on optimized SP-Rhlene only needs a cell voltage of 0.385 V at 10 mA cm−2 to generate H2, while transforming S2− into sulfur powder, which further reduces the cost of hydrogen production and protects the ecological environment. This work provides a directive strategy for the rational construction of dual heteroatom doped metallene for energy-saving hydrogen production and environmentally friendly sulfur recovery.
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Journal of Energy Chemistry
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2023
·
IF 13.1
Qiqi Mao,Wenxin Wang,Kai Deng,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts . Herein, we reported a low-content Pt-doped Rh metallene (Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen (H 2 ) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom utilization. Additionally, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of −10 mA cm −2 in the hydrogen evolution reaction (HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm −2 in the hydrazine oxidation reaction (HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage (0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm −2 for energy-saving H 2 production, which greatly reduces the electrolysis energy consumption. Moreover, DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d -band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction.
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高影响因子
IONICS
·
2023
·Vol. 29
·期 5
·1991-2003
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IF 2.8
Yuhui Cui,Jinghao Lu,Lijuan Yang,Zheng Hao,Runjin Wu,Qian Li,Shijia Xu,Libin Yang
In proton exchange membrane fuel cells (PEMFCs), the most advanced catalysts are mainly carbon loaded with platinum (Pt), but the cathodic catalytic active center is too low to match the oxidation activity and rate at the anode. Co atoms doped into the lattice of Pt alloy change the electronic structure of platinum and reduce the binding energy of oxygen atoms. Au or Rh atoms embedded into the lattice of Pt 3 Co alloy compensate the defect and enhance the activity and rate of the oxygen reduction. Through base on density functional theory (DFT), the adsorption energy for oxygen on Pt 3 Co, Au-Pt 3 Co, and Rh-Pt 3 Co and the segregation energy of Co atoms were calculated. The results show that Au or Rh doped weakens the binding energy of Pt for oxygen on the Pt 3 Co alloy and improves the activity and stability of oxygen reduction. Compared with Rh, the introduction of Au element shows better effects in the electrocatalytic reaction process. Graphical Abstract
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高影响因子
JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Yuqing Wang,Li Yan,Cunyao Li,Miao Jiang,Ziang Zhao,Guangjin Hou,Yunjie Ding
Porous organic copolymer (designated as CPOL-BP&P(OPh) 3 ) containing vinyl biphephos moieties and tris(4-vinylphenyl)phosphite (P(OPh) 3 ) moieties was synthesized through a solvothermal copolymerization technique. After metalation with Rh precursor, an efficient heterogeneous catalyst Rh/CPOL-BP&P(OPh) 3 for the hydroformylation of 1-butene is presented with high activity (TOF = 2490.3 h −1 ) and regioselectivity (l:b = 40.0). The Rh/CPOL-BP&P(OPh) 3 catalyst has been investigated by using solid-state 13 C MAS NMR, in situ FT-IR spectroscopy, nitrogen sorption measurements, SEM, TEM, and XPS. Interestingly, in situ FT-IR spectra showed that Rh species tended to coordinate with both two kinds of P species from biphephos and P(OPh) 3 ligands in the Rh/CPOL-BP&P(OPh) 3 polymer frame rather than one kind of them. Therefore, the synergistic effect of three kinds of coordination compound formed between Rh species and both ligands could be responsible for the high activity and regioselectivity observed in hydroformylation of 1-butene.
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高影响因子
Nanoscale Advances
·
2019
·Vol. 1
·期 10
·3941-3947
·
IF 0
Xiao Li,Yucong Yan,Yi Jiang,Xingqiao Wu,Shi Li,Jingbo Huang,Junjie Li,Yangfan Lin,Deren Yang,Hui Zhang
Hydrolysis of ammonia borane (AB) is a safe and convenient means of H2 production when efficient catalysts are used. Here we report a facile one-pot solvothermal method to synthesize Rh/WO3−x hybrid nanowires. Ultra-small Rh nanoparticles with an average size of ∼1.7 nm were tightly anchored on WO3−x nanowires. Rh/WO3−x catalysts exhibited substantially enhanced activity for hydrolytic dehydrogenation of AB under both dark and visible light irradiation conditions relative to mixed Rh nanoparticles and WO3−x nanowires (Rh + WO3−x), and Rh/C and WO3−x nanowires. X-ray photoelectron spectroscopy (XPS) analysis indicated that the synergistic effect between Rh nanoparticles and WO3−x nanowires was responsible for such an enhancement in activity. Specifically, Rh/WO3−x achieved the highest turnover frequency (TOF) with a value of 805.0 molH2 molRh−1 min−1 at room temperature under visible light irradiation. The H2 release rate as a function of reaction time exhibited a volcano plot under visible light irradiation, indicating that a self-activation process occurred in the hydrolytic dehydrogenation of AB due to additional oxygen vacancies arising from in situ reduction of WO3−x nanowires by AB, and thus an enhanced localized surface plasmon resonance (LSPR). Such a self-activation process was responsible for the enhanced catalytic activity under visible light irradiation relative to that under dark conditions, which was supported by the lower activation energy (45.2 vs. 50.5 kJ mol−1). In addition, Rh/WO3−x catalysts were relatively stable with only little loss in activity after five cycles due to the tight attachment between two components.
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PubMed
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Junlu Bi,Xuejun Zhai,Guishan Liu,Jing-Qi Chi,Xuanyi Wang,Shaojin Chen,Zhenyu Xiao,Lei Wang
Searching for highly efficient and Pt-free electrocatalysts with comparable hydrogen evolution reaction (HER) activities to the benchmark Pt/C catalyst is highly demanded for developing renewable water electrolysis system but still remains challenging. In the current work, low loading of P modified ultrafine Rh nanoparticles encapsulated in N, P dual-doped carbon layers (Rh–P@NPC) have been prepared through a facile polymerization-impregnation followed by high-temperature pyrolysis process . Benefiting from the unique core-shell structural advantages and synergistic effect of Rh–P and NPC components, the resulting Rh–P@NPC catalyst not only exhibits remarkable electrocatalytic activity for HER in the whole pH range with a low overpotential of 31 mV, 65 mV, and 130 mV to drive a current density of 10 mA cm −2 in 0.5 M H 2 SO 4 , 1.0 M KOH, and 1.0 M PBS , respectively, but also demonstrates high durability. It is worth to note that all these HER performances are on a par with commercial Pt/C catalysts for HER. This synthetic strategy provides possibility for the fabrication of carbon-based heterostructures with high catalytic activity and durability in harsh environments.
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高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Lin-Chang Liu,Hong-Lin Zhu,Yue-Qing Zheng
Ammonia borane (NH3BH3, referred to as AB) hydrolytic dehydrogenation is regarded as a feasible strategy for hydrogen production owing to its high hydrogen content, pollution-free nature, and high stability. Metal nitrogen-doped carbon materials (M-N-C) are considered as an ideal candidate support of catalysts with AB hydrolytic dehydrogenation due to the advantages of low cost, large specific surface area, rich defective site, and good chemical stability. In this work, tubular Ni@Ni-N-C was successfully synthesized by high-temperature pyrolysis, and then, Rh nanoparticles were decorated on the support Ni@Ni-N-C by impregnation and reduction to prepare a series of Rh/Ni@Ni-N-C. The best catalytic performance of catalysts is obtained using Ni@Ni-N-C with an Rh loading of 0.74 wt %, showing a turnover frequency as high as 782.18 min–1 and an apparent activation energy (Ea) as low as 25.86 kJ mol–1, which could be attributed to the strong interaction between Rh and the defective site of the support.
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