INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
BingBing Wang,Jian-Zhong Xu,Shuai Liu,Zhi-Ming Rao,Wei-Guo Zhang
L-Tryptophan hydroxylation catalyzed by tryptophan hydroxylase (TPH) presents a promising method for synthesizing 5-hydroxytryptophan (5-HTP), yet the limited activity of wild-type human TPH2 restricts its application. A high-activity mutant, MT10 (H318E/H323E), was developed through semi-rational active site saturation testing (CAST) of wild-type TPH2, exhibiting a 2.85-fold increase in k cat / K m over the wild type, thus enhancing catalytic efficiency . Two biotransformation systems were developed, including an in vitro one-pot system and a Whole-Cell Catalysis System (WCCS). In the WCCS, MT10 achieved a conversion rate of only 31.5 % within 32 h. In the one-pot reaction, MT10 converted 50 mM L-tryptophan to 44.5 mM 5-HTP within 8 h, achieving an 89 % conversion rate, outperforming the M1 (NΔ143/CΔ26) variant. Molecular dynamics simulations indicated enhanced interactions of MT10 with the substrate, suggesting improved binding affinity and system stability. This study offers an effective approach for the efficient production of 5-HTP.
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ChemistrySelect
·
2024
·Vol. 9
·期 21
·e202304264
·
IF 1.9
Haoyu Liu,Guoliang Zhang,Hong Yuan
Graphical A series of hierarchical ZSM-5 nanocrystalline aggregates (HNZ-5) was synthesized for the catalytic cracking of model waste cooking oil model compound (WCOMC) to produce light olefins. A series of hierarchical ZSM-5 nanocrystalline aggregates (HNZ-5) was synthesized using a hydrothermal method with tetrapropylammonium hydroxide as a structural guide. The HNZ-5 samples having different Si/Al molar ratios all showed suitable hierarchical architectures and the maximum surface area was found to be 329 m 2 /g. The SEM image displayed the width of the individual crystal particles was ~100 nm, and its nanocrystalline clusters generated intercrystalline pores. Temperature-programmed desorption with NH 3 indicated that the total acidity of this material increased with increases in the Al 3+ content to a maximum of 0.47 mmol/g at a Si/Al ratio of 15. In addition, 27 Al magic angle spinning nuclear magnetic resonance spectra showed that the acid sites were associated with tetrahedral and octahedral Al sites. This HNZ-5 was applied to the catalytic cracking of waste cooking oil model compound and gave a light olefin yield as high as 43.9 % at 550 °C. Extending the reaction time to 6000 min provided a yield of light olefins in excess of 30 %, which was higher than that achieved using traditional ZSM-5. These data confirmed that the hierarchical pore structure of HNZ-5 resulting from the self-assembly of nanocrystals, together with exposed acidic sites, promoted the catalytic conversion of large molecules.
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Xi-Lai Liu,Wei Zhong,Yu-Fan Jin,Tian-Jiao Wang,Xue Xiao,Pei Chen,Yu Chen,Xuan Ai
The electrochemical hydrogenation (ECH) of 5-hydroxymethylfurfural (HMF) to 2,5-dihydroxymethylfuran (DHMF) represents a pivotal pathway for the electrocatalytic upgrading of biomass-based organic small molecules, offering significant reductions in energy consumption while producing value-added chemicals. The conversion of HMF to DHMF is challenging due to the high reduction potential and complex intermediates of HMF ECH under neutral environment. Also, the total efficiency is hindered by sluggish anodic oxygen evolution reaction (OER) kinetics. Herein, we report a synthesis of highly alloyed Pd-Pt bimetallene (Pd 3 Pt 1 BML) for HMF ECH coupled with formic acid oxidation reaction (FAOR). Through a combination of in-situ Raman spectroscopy, electron paramagnetic resonance analysis, and theoretical calculations, we elucidate that the HMF adsorption on Pd atoms, strategically separated by Pt atoms, is weakened compared to pure Pd surfaces. Additionally, Pt atoms serve as crucial providers of active hydrogen to neighboring Pd atoms, synergistically enhancing the reaction kinetics of HMF conversion with a Faradaic efficiency >93%. Meanwhile, the atomically dispersed Pt atoms endow Pd 3 Pt 1 BML with high electrochemical performance for the direct pathway of FAOR at the anode. As a result, a FAOR-assisted HMF ECH system equipped with bifunctional Pd 3 Pt 1 BML achieves the energy-efficient conversion of HMF to DHMF at electrolysis voltage of 0.72 V at 10 mA cm –2 . This work provides insights into the rational design of bifunctional catalysts featuring two distinct types of active sites for advanced energy electrocatalysis and ECH.
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JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
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2024
·Vol. 39
·期 2
·332-336
·
IF 1.3
Ma Kuoyan,Zhao Pengxian,Yi Hongyu,Yu Haijun,Zhou Moxi,Zhang Lingling,Liu Yupu
A core-shell composite consisting of ZSM-5 zeolite as the core and ordered mesoporous silica as the shell was prepared by a surfactant-controlled sol-gel process and using tetradecylamine (TDA) as the template and Tetraethylorthosilicate (TEOS) as the silica precursor. The pores of the silica shell were found to be ordered and perpendicular to the crystal faces of the zeolite core. The thickness of the shell in the core-shell structured composite can be adjusted in the range of 20–90 nm, while the surface morphology and the pore size distribution were modified by changing the mass ratio of TEOS to zeolite. The composite molecular sieves have higher surface area for capturing molecules than ZSM-5, and with the increase of mesoporous shell layer, the ZSM-5@SiO 2 - x composites show stronger adsorption capacity of butyraldehyde. However, when the shell thickness exceeds 90 nm, the adsorption capacity of butyraldehyde decreases instead. The composites have a huge potential for environmental applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
·
IF 3.8
Wenxuan Zhang,Chuqian Xiao,Yuhang Li,Chunzhong Li
5-Hydroxymethylfurfural (HMF) electrooxidation for 2,5-furandicarboxylic acid (FDCA) production has become a sustainable method for value-added products at the anode. Here, an amorphous NiMo composite oxide supported on nickel foam (NF) is fabricated for HMF electrooxidation (HMFOR) via one-step electrodeposition. The synthesized NiMo/NF delivers 98.3% FE toward FDCA at 1.5 VRHE and maintains FE above 90% during 10 h. In situ Raman spectroscopy proves the formation of the active species Ni3+-OOH during the reaction process. Due to the introduction of high-valent Mo6+, the Ni3+ active species can be stabilized and the adsorption of aldehyde in HMF can be promoted during the reaction process, thus enhancing the FDCA electrosynthesis performance.
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STAR Protocols
·
2024
·
IF 1.3
Wenbin Zhang,Felix Ofori Boakye,Guanwu Lian,Dingyi Zhang,Zhousheng Mo,Henan Chen,Baiyao Liang,Yun Zhang,Wei Zhao
Summary Recently, there has been a growing interest in using sustainable energy to decrease lignin monomers to generate high-value-added products. Here, we present a protocol for electrocatalytic hydrogenation of 5-hydroxymethylfurfural. We describe steps for catalyst preparation, performing electrocatalytic experiments, high-performance liquid chromatography analysis, and in situ infrared reflection-absorption spectroscopy testing. The synthesized catalyst used in this reaction exhibits enhanced selectivity and Faradaic efficiency in NaClO 4 solution. For complete details on the use and execution of this protocol, please refer to Zhang et al. 1
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Molecular Catalysis
·
2024
·
IF 3.9
Zhijiao Huang,Yong Liu,Lungang Chen,Xinghua Zhang,Jianguo Liu,Chenguang Wang,Qi Zhang,Longlong Ma
2,5-dimethylfuran (DMF), a promising biomass-derived fuel, is synthesized via the hydrodeoxygenation of 5-hydroxymethylfurfural (HMF). This study focuses on the inherent activity of a 5Pt5Fe/C catalyst for HMF hydrodeoxygenation to DMF. The catalyst exhibited exceptional performance, achieving a remarkable DMF yield of 99.6 %. It displayed specific selectivity for C = O bond hydrogenation and C O bond cleavage in diverse substrates, producing high yield of 2-methylfuran from furfural and furfury alcohol, and high yield of toluene from benzaldehyde, benzyl alcohol. In-depth characterizations unveiled valuable insights into the 5Pt5Fe/C catalyst's properties, emphasizing a harmonious balance between metal and acid sites due to the interactive synergy between Pt and Fe species, enhancing hydrodeoxygenation activity. Additionally, the catalyst demonstrated satisfactory stability, maintaining a commendable DMF yield over five reaction cycles despite observed changes.
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CRYSTENGCOMM
·
2024
·Vol. 26
·期 21
·2775-2783
·
IF 2.6
Yaqoot Khan,Ismail Ismail,Hongwei Ma,Zhongkui Li,Hui Li
Hydrogen bonds are the fundamental factors stabilizing DNA and RNA macromolecules. Based on their base-pair sequences, DNA and RNA perform various biological functions. A key feature of these sequences is their linkage via hydrogen bonds. The hydrogen bonding between sugars and nucleobases in RNA sequences is one of the major reasons behind several mutagenic disorders that can cause numerous genomic instabilities, various genetic diseases, and RNA rearrangement problems. Chemists explore hydrogen bonding stability in nucleic acids, which is crucial for understanding molecular-level differentiations with potential applications in the early diagnosis of hereditary diseases. In this work, five types of coordination polymers of CMP and dCMP, {[Cd(CMP)(bpa)(H2O)3]·2H2O}n (1), {[Cd(dCMP)2(bpa)(H2O)2]·4H2O}n (2), {[Cd(azpy)(H2O)4](CMP)·3H2O}n (3), {[Cd(dCMP)2(azpy)(H2O)2]·4H2O}n (4), and {[Cd(CMP)(bpe)(H2O)3]·2H2O}n (5) (azpy = 4,4′-azopyridine, bpa = 1,2-bis(4-pyridyl)ethane, and bpe = 1,2-bis(4-pyridyl)ethylene), were designed and studied. All complexes were fully characterized by employing the single-crystal X-ray diffraction method. Complex 1 is a 2D coordination polymer, whereas complexes 2–5 are 1D coordination polymers. Significantly, a novel sugar–nucleobase hydrogen bonding interaction was discovered in complexes 1, 3, and 5 for the first time, thus introducing a new supramolecular interaction that can be used in self-assembly and molecular recognition. The chirality in the supramolecular assemblies of the five complexes was comprehensively analyzed using single-crystal and solid-state CD spectra.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Haodong Zheng,Xiaoxiang Wang,Kaile Shi,Yidong Hu,Wenxuan Lv,Pengfei Yin,Chengze li,Libo Sun,Jingjing Wang,Boxiong Shen,Hui Liu
Electrochemical organic oxidation has shown great industrial potential due to its green, low-carbon, and energy-efficient advantages. However, the competing oxygen evolution reaction (OER) severely impacts the faradaic efficiency and conversion rate of organic oxidation reactions. In this work, we report a method that can promote the oxidation of 5-hydroxymethylfurfural (HMFOR) while suppressing the OER, which is achieved by etching NiMnFe-LDH with N,N-dimethylacetamide (DMF), resulting in the formation of numerous cationic defects. Specifically, at a current density of 50 mA cm–2, the applied potential for HMFOR decreased by 50 mV, while the OER potential increased by 30 mV. In situ electrochemical impedance spectroscopy found faster reaction kinetics for d-NiMnFe-layered double hydroxide (LDH) compared to that of NiMnFe-LDH in HMFOR, whereas an opposite trend was observed in the OER, confirming that the DMF treatment has opposite effects on the transportation of organic molecules and OH–. To further investigate the reaction pathways and evolution of intermediates during HMFOR, in situ infrared spectroscopy and theoretical calculations were conducted, which demonstrate that cationic defects not only significantly enhance the adsorption of intermediates but also lower the reaction energy barrier, thus accelerating the reaction rate of HMFOR. This work provides a potential strategy for developing industrial-grade electrocatalysts for high current densities.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Shuai Liu,Wenting Cai,Tongxue Zhang,Ke Fan,Xijun Liu,Xubin Zhang,Fumin Wang
The electrocatalytic stabilization of 5-hydroxymethylfurfural oxidation reaction (HMFOR) alongside hydrogen production offers an effective and cost-efficient approach to attaining a zero-carbon economy. Nickel-based electrocatalysts are viable options owing to their intrinsic redox properties; yet, HMFOR entails many hydroxide ions (OH-) and multi-electron synergistic catalytic mechanisms in alkaline electrolytes. The limited OH- capture capacity of nickel-based catalysts results in diminished energy conversion efficiency. Furthermore, the inadequate intrinsic catalytic activity of nickel and its propensity to reorganize into a singular hydroxide at elevated potentials results in aggregation. To tackle these issues, we developed a new catalyst (Co-NiO/Cr2O3) employing an approach that integrates heteroatom doping and microenvironment engineering. Experimental data indicate that this catalyst attains a Faradaic efficiency of 99.2% and a selectivity for 2,5-furan dicarboxylic acid (FDCA) of 99.17%. The doping of cobalt precisely modulates the coordination environment of nickel, whereas Cr2O3 serves as a quintessential Lewis acid, with its surface Cr3+ sites exhibiting a robust ability to receive electron pairs, thereby accumulating hydroxide ions from the solution and establishing a localized basic environment at the active sites. This work presents an innovative and effective HMFOR catalyst while also proposing a new approach for the design and development of catalysts for value-added biomass conversion.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xitong Yang,Ruifeng Zhou,Guowei Liu,Sajjad Hussain,Qiuye Li
Catalytic regeneration has become one of the most promising technologies to solve the high energy consumption problem of CO 2 capture in organic amine solutions. As the most mainstream type of catalyst, the instability of acidic catalysts in alkaline solutions attracts increasing attention from researchers. Herein, we proposed a composite catalyst of MnOOH loaded HZSM-5 to weaken the adsorption of alkaline substances and improve the catalytic stability of the catalytic material. The optimized catalytic effect is obtained when the mass ratio of MnOOH is 20% The CO 2 desorption efficiency is increased by 68.2%, and the energy consumption is reduced by 31.8% when the dosage of the catalyst is only dosage of 0.2 wt% amine solution. Through materials characterization and DFT calculations, it was found that the surface O and hydroxyl groups on MnOOH are the key factors for proton cycling, and HZSM-5 has an important impact on improving proton transfer rate. This work provides a valuable approach to solving the stability problem of acidic catalysts.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2025
·
IF 6.2
Shuang Du,Nan Zheng,Zehua Zhang,Chenhao Zhang,Huimin Zhou,Yu Deng,Jian Yin,Yongchao Cai,Xiaole Xia
5-Aminolevulinic acid synthase (ALAS) is the key rate-limiting enzyme in the synthesis of the vital biosynthetic intermediate 5-aminolevulinic acid (ALA). However, its catalytic efficiency is compromised due to its low activity and poor stability. Here, we obtained the mutant I325M/V390Y/H391I (T6), which exhibited a 7.0-fold increase in specific activity (2.53 U/mg) compared to the wild type through the application of isothermal compressibility (βT) perturbation engineering in conjunction with two thermal stability prediction algorithms. Moreover, molecular dynamics simulations indicate that positive changes in intermolecular interactions, the substrate channel, and the binding pocket account for the improved catalytic activity of T6. Furthermore, T6 was immobilized on magnetic chitosan nanoparticles, maintaining 73.5% of its original activity after 10 reaction cycles. Overall, combination approaches were employed to construct a superior ALAS variant, providing a novel concept for the synthesis of ALA and a valuable benchmark for optimizing industrial enzymes in related fields.
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