Molecular Catalysis
·
2024
·
IF 3.9
Wenhao Xia,Shimeng Liu,Lihui Huang,Hao Wu,Tao Bai,Shanshan Wang,Fei Hao,Xiao Wang,Wen Wang
d -tagatose, a rare sugar with broad applications in the food and pharmaceutical industries, can be synthesized from d -fructose by epimerases, an approach with significant biosynthesis potential. However, so far there has been only one attempt to engineer tagatose 4‑epimerase through random mutagenesis. The lack of exploration has severely restricted the application of epimerases in the industrial production of d -tagatose. The previous research primarily focused on enhancing the catalytic activity of epimerases through random mutagenesis, with limited understanding of how substrate-adjacent residues affect enzyme efficiency, which was hence the subject of this study. First, using a semi-rational design approach, after three rounds of mutagenesis and screening, the mutant (S125D/S268A/Q124E) of D-tagaturonate epimerase (UxaE) from Thermotoga neapolitana was obtained, which increased d -tagatose production efficiency by 10.8-fold compared to the wild type, with a specific activity of 1505.6 U/g, representing the highest specific activity reported for a UxaE mutant to date. Molecular dynamics simulations showed that the substitution of Ser to Asp-125 enhanced substrate-enzyme interactions, while the substitution of Glu to Gln-124 reinforced the hydrogen bond network around the catalytic residue Glu-128, further reshaping the substrate-binding pocket and enhancing catalytic activity. This study for the first time explored the enhancement of the C4 epimerization function of epimerases by reshaping their substrate-binding pockets, thereby providing a feasible route for the industrial biosynthesis of d -tagatose.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yong Chen,Zhao Yang,Yunbo Liu,Yong Liu
In this paper, a novel Fenton-like system was constructed by a new catalyst (CNTs-Fe-Cu) combined with Al 0 -CNTs to in situ generate H 2 O 2 from activating O 2 for the degradation of sulfamerazine (SMR). The CNTs-Fe-Cu composite was prepared and characterized by XRD, SEM, EDS and BET methods. The results showed that H 2 O 2 could be generated in-situ by Al 0 -CNTs composite under oxygen aeration, which was then converted to OH and O 2 − radical by CNTs-Fe-Cu composite. The high removal efficiency of SMR could be obtained in Al 0 -CNTs/CNTs-Fe-Cu/O 2 system at a relatively broad range of pH. Furthermore, the removal efficiency of SMR and total organic carbon (TOC) was 85% and 60%, respectively under the following condition: initial pH = 5.8, T = 25 °C, O 2 flow rate = 400 mL/min, CNTs-Fe-Cu = 1 g/L, Al 0 -CNTs = 1 g/L, SMR = 50 mg/L, reaction time = 60 min. In addition, the intermediate products of SMR degradation were identified and the possible degradation pathways of SMR and the degradation mechanism of Al 0 -CNTs/CNTs-Fe-Cu/O 2 process were tentatively proposed.
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 10
·3121-3130
·
IF 7
Qian-Qian Chen,Chun-Li Hu,Bing-Xuan Li,Jiang-Gao Mao
Exploration of new iodates is crucial due to their splendid applications in the nonlinear optical (NLO) field. Two new IIIA metal iodate–selenates, namely, [M(OH)2]3(IO3)(SeO4)·H2O (M = Ga and In), have been successfully synthesized using the hexagonal tungsten oxide (HTO) framework as an ideal structural template. Isostructural [M(OH)2]3(IO3)(SeO4)·H2O (M = Ga and In) crystallize in the polar space group P63mc. Their structures feature ∞[MO2(OH)2]3− (M = Ga, In) layers composed of corner-shared circular M3O6(OH)9 trimeric units based on MO2(OH)4 octahedra. The SeO4 groups are capped above half of the trimeric units of the layers while the IO3 groups are capped below the remaining trimeric units of the layers. Both compounds exhibit moderate phase-matchable second-harmonic generation (SHG) responses (2.9× and 3.8× KH2PO4) under 1064 nm laser radiation and the same band gap of 3.38 eV. Results of theoretical calculations revealed that their SHG effects originated from the synergistic effect of MO6, IO3 and SeO4 groups. So far reports on iodate–selenates are scarce and this work provides a new perspective to design new NLO materials through polar HTO-type topologies and a mixed-anionic strategy.
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Fang Li,Pengfei Du,Haili Lin,Huiqin Yu,Yang Wang,Bin Fang,Jing Cao
Replacing the anodic oxygen evolution reaction with electro-oxidation of glycerol for hydrogen energy not only reduces energy consumption but also obtains high-value chemicals. However, this system still faces bottlenecks of limited Faradaic efficiency, low selectivity, and an unclear reaction pathway. Herein, the Mott–Schottky Ni(OH)2–In heterostructure was prepared for selective glycerol electro-oxidation (GOR). A series of experiments and theoretical calculations validated the charge shuttling through a heterointerface and the formation of the built-in electric field (BIEF) structure. As expected, the Ni(OH)2–In delivered a low potential of 1.22 V vs RHE at 10 mA cm–2. The Faradaic efficiency and selectivity for formate are up to 93% and 95%, respectively, together with long-term stability for the 20 cycles. The excellent performance can be attributed to the changed reaction pathway of producing the formate, reduced reaction energy barrier of the rate-determining step (RDS), and a more rapid GOR kinetics which arise from the robust BIEF. This work indicates that via constructing BIEF in the Mott–Schottky heterostructure, the electrocatalytic glycerol oxidation can be promoted.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Qingli Xu,Wenluan Gao,Miao Wang,Gang Yuan,Xiaona Ren,Rong Zhao,Sida Zhao,Qingfa Wang
To develop earth-abundant and cost-effective catalysts for overall water splitting is still a major challenge. Herein, a unique “raisins-on-bread” Ni–S–P electrocatalyst with NiS and Ni 2 P nanoparticles embedded in amorphous Ni(OH) 2 nanosheets is fabricated on Ni foam by a facile and controllable electrodeposition approach. It only requires an overpotential of 120 mV for HER and 219 mV for OER to reach the current density of 10 mA cm −2 in 1 M KOH solution. Employed as the anode and cathode , it demonstrates extraordinary electrocatalytic overall water splitting activity (cell voltage of only 1.58 V @ 10 mA cm −2 ) and ultra-stability (160 h @ 10 mA cm −2 or 120 h @50 mA cm −2 ) in alkaline media . The synergetic electronic interactions, enhanced mass and charge transfers at the heterointerfaces facilitate HER and OER processes. Combined with a silicon PV cell, this Ni–S–P bifunctional catalyst also exhibits highly efficient solar-driven water splitting with a solar-to-hydrogen conversion efficiency of 12.5%.
✓ 已验证
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2024
·Vol. 137
·期 3
·1635-1649
·
IF 1.7
Pan Weixing,Chen Hui,Chen Aicheng
A series of low-cost α-Ni(OH) 2 /SiO 2 catalysts were successfully fabricated by the vapor-induced internal hydrolysis method, then the hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (BHMF) was investigated by using the ethanol as the hydrogen donor over these as-prepared α-Ni(OH) 2 /SiO 2 catalysts. Based on the reaction results, these as-prepared catalysts, which could dispense with extra pre-reduction treatment before reactions, exhibited superior catalytic performance for the HMF hydrogenation to BHMF. A remarkable intrinsic selectivity of BHMF selectivity of almost 100% with about 90% HMF conversion could be obtained under 195 °C for 5 h in an N 2 atmosphere over the α-Ni(OH) 2 /SiO 2 catalyst of 5-Ni(OH) 2 /SiO 2 with about 5 wt% Ni on SiO 2 . The almost constant HMF conversion and BHMF intrinsic selectivity found from the recycling tests can indicate that the catalyst was stable without the obvious loss of its catalytic activity after recycling. Moreover, the mechanism of HMF hydrogenation using ethanol over the α-Ni(OH) 2 /SiO 2 catalysts could be referred to as the mechanism of the Meerwein-Ponndorf-Verley reaction. This work will provide a simple synthesis method for future design and development of high-performance, low-cost, and low-energy consumption catalysts for HMF hydrogenation to BHMF.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jiawen Wu,Xiaonan Sun,Junting Wu,Xue Yu
This study proposes a green and simple strategy for efficiently removing heavy metals from wastewater by activating biochar with eggshell and in-situ generating CaO/Ca(OH) 2 . Characterization results revealed that the composite carbon material (BCEg15) successfully incorporated CaO/Ca(OH) 2 active sites compared to the raw biochar (BC). Additionally, eggshell activation increased the specific surface area and pore volume of BCEg15 by 4.36 and 6.80 times, respectively, compared to BC. These structural enhancements increased the maximum adsorption capacity of BCEg15 for Pb 2+ and Cd 2+ by 20.68 and 42 times, respectively, compared to BC. Importantly, the loading of CaO and Ca(OH) 2 significantly enhanced the ion exchange and mineral precipitation capacities of the biochar. For instance, compared to BC, the adsorption capacities of BCEg15 attributed to ion exchange (Q e ) for Pb 2+ and Cd 2+ rose by 403.12 mg/g and 197.65 mg/g, respectively, while the adsorption capacities attributed to mineral precipitation (Q p ) increased by 19.60 times and 45.20 times, respectively. BCEg15 demonstrated excellent reusability, maintaining adsorption capacities of 461.18 mg/g for Pb 2+ and 265.26 mg/g for Cd 2+ after five cycles. Additionally, BCEg15 outperformed commercial activated carbon in treating heavy metals from desulfurization wastewater from coal-fired power plants, achieving a removal efficiency of 99.98 % compared to 48.22 %. The primary mechanisms by which BCEg15 removes Pb 2+ and Cd 2+ were identified as ion exchange, mineral precipitation, complexation with oxygen-containing functional groups, and interactions with π electrons. Density functional theory (DFT) was utilized to delve deeper into the microscopic mechanisms of adsorption. The findings showed that the O-top site of CaO exhibited the greatest stability for heavy metal adsorption. Electron density difference maps and partial density of states (PDOS) results revealed a denser electron cloud and greater orbital overlap between CaO and Pb 2+ compared to Cd 2+ , suggesting a higher affinity and adsorption capacity for Pb 2+ , consistent with the experimental findings. This study presents an effective method for preparing adsorbents capable of removing Pb 2+ and Cd 2+ from wastewater and offers theoretical insights into the adsorption mechanisms of metal oxide-incorporated biochar.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Jun Ma,Pengsong Li,Xiao Lin,Yijun Huang,Yang Zhong,Lipeng Zhang,Xiaoming Sun,Daojin Zhou,Wen-Feng Lin,Zhenhai Xia
Developing low-cost yet highly efficient earth-abundant electrocatalysts for oxygen evolution reaction (OER) is of great significance for industrial scale water splitting for clean hydrogen production, as well as for rechargeable metal-air batteries. In searching for advanced catalysts, it is equally important to fundamentally understand working mechanism and be able to rationally design and manipulate catalytic sites. Starting from the density functional theory (DFT) calculations as a guidance, our theoretical model revealed that chromium substitution in nickel–iron hydroxides (Ni 1-x Fe x (OH) 2 ) not only accelerated the charge transfer but also regulated the adsorption energy of OER intermediates to achieve optimal binding strength. Experimentally, chromium was doped into the laminate of Ni 1-x Fe x (OH) 2 , resulting in the enhanced catalytic performance for oxygen evolution reaction, which confirmed the predictions from the theoretical data. The porous and ultra-thin ternary Ni 1-x-y Fe x Cr y (OH) 2 electrocatalysts were grown directly on a nickel foam (NF) substrate, with an optimum composition Ni 0.66 Fe 0.27 Cr 0.07 (OH) 2 /NF identified, which exhibited a superior OER performance, i.e., achieving a significant current density of 10 mA cm −2 at a low overpotential of 231 mV, a small Tafel slope (31 mV dec −1 ) and an excellent stability at a highly oxidative potential of 1.68 V vs RHE in alkaline electrolyte. The comprehensive study involving both theoretical and experimental results in this work provides an insightful guidance in designing efficient OER catalysts for chemical and electrical energy conversion and storage.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Yifan Ma,Wei He,Youyu Duan,Yang Wang,Yuhan Li,Fan Dong
Oxygen vacancies induce charge redistribution, facilitating oxygen adsorption. • S-scheme heterojunctions enable efficient charge separation while retaining high redox potential. • The dual-electron transfer pathway facilitates the rapid electron transfer to O 2 . • Lowered thermodynamic barrier of the rate-determining step by modulation of ROSs generation. Transition metal stannates are promising for efficient air purification due to their remarkable activity in volatile organic compounds (VOCs) degradation. However, the interfacial charge-transfer behavior and the fundamental mechanism of aromatic ring activation, specifically, C-H bond cleavage and ring-opening oxidation remain elusive, hindering rational catalyst design for toluene (C 7 H 8 ) mineralization. Herein, an oxygen-vacancy-enriched S-scheme heterojunction (SMSH-30) is constructed via a facile one-step hydrothermal strategy. The optimized heterostructure exhibits outstanding toluene removal (96.65%), mineralization efficiency (101.8%), and long-term stability (>600 min). Combined experimental and theoretical analyses unveil that oxygen vacancies (OVs) modulate charge transfer and reactive oxygen species (ROS) evolution: (1) OVs induce dual-channel electron migration, greatly facilitating interfacial charge transfer; (2) this enhanced transfer promotes O 2 activation into highly oxidative singlet oxygen ( 1 O 2 ); and (3) the optimized interface accelerates intermediate conversion with a favorable Gibbs free energy profile. This work provides molecular-level insights into charge dynamics and ROS modulation within S-scheme heterojunctions, offering a new paradigm for rational design of advanced photocatalysts toward deep VOC mineralization and sustainable air purification. Download: Download high-res image (156KB) Download: Download full-size image Combined experimental characterizations and density functional theory calculations revealed that oxygen vacancies serve as continuous O 2 activation centers, while the S-scheme interface promotes efficient charge separation and preserves high-redox-potential electrons for singlet oxygen generation toward complete anti-poisoning mineralization of toluene.
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Dongming Li,Weixin Li,Daheng Wang,Xuan He,Xing Du,Hui Chen,Wei Fang,Haijun Zhang,Cheng Gong,Lei Zhao
Electrocatalytic water splitting technology is pivotal for building a green and sustainable society. However, practical application has been hindered by insufficient catalyst activity, leakage risks of liquid electrolytes, and interfacial mass transfer limitations. Herein, we designed an electrocatalytic water-splitting device comprising a superhydrophilic/superaerophobic 6‑nickel (II) hydroxide supported on materials of institute lavoisier-100 (Fe) (6-Ni(OH) 2 /MIL-100) catalyst paired with cobalt-modified polyacrylic acid sodium salt (Co-PAAS) hydrogel featured with high ionic conductivity. Through the construction of size-gradient hierarchical pore channels, water directionally transports from the Co-PAAS hydrogel to 6-Ni(OH) 2 /MIL-100, significantly reducing interfacial impedance. The 6-Ni(OH) 2 /MIL-100 catalyst achieves a low overpotentials of 133 mV for the oxygen evolution reaction (OER) and 190 mV for the hydrogen evolution reaction (HER) at 50 mA cm −2 in 1.0 M KOH, with an overall water-splitting cell voltage of 1.520 V. It demonstrates stable operation for 40 h at 1000 mA cm −2 . The Co-PAAS hydrogel exhibits a maximum moisture uptake of 0.40 g g −1 and an exceptional ionic conductivity of 83.3 mS cm −1 . The integrated quasi-solid-state electrolyzer, combining Co-PAAS hydrogel and 6-Ni(OH) 2 /MIL-100, requires only 1.475 V at 50 mA cm −2 and maintains a current density decay rate < 5% after 400 h of continuous operation. This work provides a transformative strategy and theoretical foundation for industrial and portable electrocatalytic water-splitting technology.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xinyuan Wei,Junyan Wei,Jianqiao Xu,Qing Zheng,Xiaolei Teng,Zunyao Wang,Ruijuan Qu
The generation of highly reactive hydroxyl radicals (•OH) in natural water under sunlight irradiation has been demonstrated to significantly affect the degradation of compounds in water. However, studies concerning the effects of free •OH on the degradation of hydrophobic pollutants in real, complex environments remain limited. This study examined how •OH generated by a UV/H₂O₂ system affects the heterogenous photodegradation of polychlorinated biphenyls (PCBs) in a natural suspended particle-water system. The results showed that •OH effectively decomposed PCB-3, 15 and 47, but had no effect on PCB-136, 155, 206 and 209. Further experiments revealed that •OH in the aqueous phase primarily reacts with PCBs that have desorbed into the water. The short diffusion distance of •OH and the higher potential energy barriers in hydrophobic regions hindered its reaction with PCBs on particle surfaces. Lowering solution pH or adding certain cations improved PCB-3 degradation by increasing its aqueous partitioning. Conversely, the presence of humic acid (HA) could quench •OH and screen light, thereby hindering the degradation of PCB-3 on particle surface by •OH. This study provides valuable insights into the mechanisms of •OH mediated degradation of hydrophobic pollutants and may advance the development of environmental treatment technologies.
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 7
·1-14
·
IF 2.4
Li Shunming,Hu Pengyu,Qu Jingzong,Zhou Jie,Wang Zibo,Wang Yanan,Sun Tao,Chen Anran
Hydrogen evolution reaction (HER) in alkaline media demands cost-effective and highly active electrocatalysts to replace noble metals. Herein, we report a ternary MoS₂/Ni₃S₂/Ni(OH)₂ nanoflower composite supported on nickel foam (NF) via a facile one-step electrodeposition strategy. This method enables precise control of MoS₂ morphology while mitigating aggregation-induced active site blockage. The synergistic interplay among MoS₂ (exposing edge sites), conductive Ni₃S₂, and Ni(OH)₂ (modulating electronic structure) significantly enhances HER kinetics. Notably, the optimal catalyst (5-min deposition) achieves ultralow overpotentials of 48 mV at 10 mA cm⁻² and 175 mV at 100 mA cm⁻² in 1.0 M KOH, surpassing most reported Ni- or Mo-based catalysts. Furthermore, it exhibits exceptional stability with negligible activity loss after 5000 cycles and 72-hour continuous operation. XPS analysis reveals that a high Mo⁴⁺/Mo⁶⁺ ratio facilitates electron delocalization, accelerating hydrogen intermediate desorption. This work establishes a new paradigm in HER catalyst design through interface-engineered ternary systems. By unifying electronic synergy theory with the SPRE synthesis method, we overcome the activity-stability trade-off plaguing binary catalysts. The demonstrated 500-hour stability at industrial current densities (100 mA cm⁻²) positions this approach as a transformative solution for scalable green hydrogen production. Graphical
✓ 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）