ACS Catalysis
·
2026
·
IF 13.6
Wang Kaixin,Dang Shanshan,Tong Qi,Gao Peng,Ni Xiaolu,Zhang Zhenzhou,Tu Weifeng
Although industrial Cu/ZnO/Al 2 O 3 catalysts are highly promising for methanol synthesis from CO 2 hydrogenation, identifying the nature of the surface active structure and establishing a quantitative structure-activity relationship remain elusive. Herein, through integrated qualitative, titration, and isothermal adsorption characterizations, we elucidate how Zr species promotion tailors the electronic and structural properties of Cu/ZnO x interfacial sites—the primary active sites. A substantial methanol STY of 0.813 g g cat –1 h –1 is achieved over the Cu/ZnO/Al 2 O 3 -2Zr catalyst at 503 K and 3 MPa with an H 2 /CO 2 ratio of 4 and a GHSV of 40,000 mL g cat –1 h –1 , a 23.9% leap over the pristine benchmark. Mechanistically, a linear dependence of CO 2 conversion on the density of Cu/ZnO x interfacial sites is established, which originates from the improved dispersion of both ZnO and Cu induced by moderate ZrO 2 incorporation. Electronic analyses reveal that Zr species acts as an electron donor to ZnO x , enriching its electron density. This electronic modulation facilitates H 2 dissociation and the surface Zn-H-Zn species formation even at low temperature, selectively driving the intermediate hydrogenation to methanol. In situ spectroscopies identify a sequential HCOO* → CH 3 O* hydrogenation pathway for methanol synthesis. Ultimately, this work establishes a definitive quantitative structure-activity relationship, paving a clear path for designing advanced industrial methanol catalysts.
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INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
·
2026
·
IF 4.7
Tao Guo,Qiulin Niu,Lu Jing,Tao Zhong,Chenyi Zhu,Binghui Wu,Shengfeng Zhang,Shibo Guo
To improve h-BN dispersion and the local interfacial environment in WC-based cemented carbides, an h-BN@Al₂O₃ composite powder was prepared by heterogeneous nucleation and calcination, with h-BN as the designed core phase and Al₂O₃ as the designed outer-layer component. The composite powder was incorporated into WC-based cemented carbides consolidated by spark plasma sintering (SPS), and the effects of powder content and sintering temperature on phase composition, microstructure, mechanical properties, and densification characteristics were examined. The h-BN@Al₂O₃ content was closely related to WC grain size, microstructural uniformity, and porosity. At 1300 °C, the specimen containing 5 vol% h-BN@Al₂O₃ had a fine, relatively homogeneous microstructure with few visible pores; higher additions increased porosity and local particle agglomeration. For the 5 vol% composition, raising the sintering temperature from 1100 to 1400 °C increased the relative density and reduced visible porosity. At 1500 °C, local WC grain coarsening, microstructural inhomogeneity, and residual porosity increased, accompanied by lower mechanical properties. The best overall performance was obtained with 5 vol% h-BN@Al₂O₃ at 1400 °C: a relative density of 99.1 ± 0.4%, flexural strength of 871.3 ± 26 MPa, Vickers hardness of 1912.1 ± 38 HV, and fracture toughness of 9.86 ± 0.2 MPa·m 1/2 .
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COLLOID AND POLYMER SCIENCE
·
2023
·Vol. 301
·期 11
·1285-1294
·
IF 2.4
Shi Ran,Yang Qingfeng
Gels formed by bio-macromolecules, free of any initiators, crosslinkers, and other chemical additive agents, are prospective environmentally friendly materials. In this work, organohydrogels prepared from chitosan and polyvinyl alcohol (PVA) without any chemical additive agents are fabricated based on physical crosslink approach and are endowed with anti-freezing and highly stretchable properties. The mechanical properties and phase transition behaviors are investigated. These highly-stretchable organohydrogels display obvious strain and strain rate-dependent tensile properties, where the rupture strain can reach as large as ~ 17. The samples show reversible elasticity at small strains and irreversible plasticity at large strains, accompanied with first a strain softening and then a strain hardening during the stretching process. The cyclic tensile tests present that the samples exhibit residual strain and hysteresis at step loadings, and the rupture behaviors strongly depend on the strain, strain rate, and waiting time. The differential scanning calorimetry (DSC) tests demonstrate that the organohydrogels present only one endothermic melting peak around 60 °C without obvious glass transitions at − 60–60 °C, indicating the stability of the anti-freezing organohydrogels at ultralow temperatures.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Liu Jianming,Zhang Han,Xu Yingying,Meng Hao,Zeng An-Ping
The use of gaseous and air-captured CO 2 for technical biosynthesis is highly desired, but elusive so far due to several obstacles including high energy (ATP, NADPH) demand, low thermodynamic driving force and limited biosynthesis rate. Here, we present an ATP and NAD(P)H-free chemoenzymatic system for amino acid and pyruvate biosynthesis by coupling methanol with CO 2 . It relies on a re-engineered glycine cleavage system with the NAD(P)H-dependent L protein replaced by biocompatible chemical reduction of protein H with dithiothreitol. The latter provides a higher thermodynamic driving force, determines the reaction direction, and avoids protein polymerization of the rate-limiting enzyme carboxylase. Engineering of H protein to effectively release the lipoamide arm from a protected state further enhanced the system performance, achieving the synthesis of glycine, serine and pyruvate at g/L level from methanol and air-captured CO 2 . This work opens up the door for biosynthesis of amino acids and derived products from air.
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Advanced Science
·
2023
·
IF 15.1
Junjie Li,Gang Wei,Gongwen Liu,Yawei Du,Ruizhi Zhang,Aifei Wang,Baoshan Liu,Wenguo Cui,Peng Jia,Youjia Xu
Postmenopausal osteoporosis is one of the most prevalent skeletal disorders in women and is featured by the imbalance between intraosseous vascularization and bone metabolism. In this study, a pH-responsive shell–core structured micro/nano-hydrogel microspheres loaded with polyhedral oligomeric silsesquioxane (POSS) using gas microfluidics and ionic cross-linking technology are developed. This micro/nano-hydrogel microsphere system (PDAP@Alg/Cs) can achieve oral delivery, intragastric protection, intestinal slow/controlled release, active targeting to bone tissue, and thus negatively affecting intraosseous angiogenesis and osteoclastogenesis. According to biodistribution data, PDAP@Alg/Cs can successfully enhance drug intestinal absorption and bioavailability through intestine adhesion and bone targeting after oral administration. In vitro and in vivo experiments reveal that PDAP@Alg/Cs promoted type H vessel formation and inhibited bone resorption, effectively mitigating bone loss by activating HIF-1 α /VEGF signaling pathway and promoting heme oxygenase-1 (HO-1) expression. In conclusion, this novel oral micro/nano-hydrogel microsphere system can simultaneously accelerate intraosseous vascularization and decrease bone resorption, offering a brand-new approach to prevent postmenopausal osteoporosis.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Siqi Tong,Dan Chen,Xinbai Jiang,Zhixiang Xu,Xiaodong Liu,Jinyou Shen
A novel composite biochar synthesized from Fenton sludge (FS) and sewage sludge (SS) was employed to catalyze persulfate for the removal of 1-H-1,2,4-triazole (TZ). The optimized conditions for the synthesis and operating process were identified through response surface methodology as follow: SS/FS mass ratio = 5:1, catalyst dosage = 0.9 g L −1 and PDS concentration = 0.5 g L −1 . The removal efficiencies of TZ, TOC and organic nitrogen were found to be as high as 97.6%, 80.33% and 100%, respectively, with the addition of Fe 3 O 4 -doped biochar in persulfate catalytic system. Besides, Fe 3 O 4 -doped biochar exhibited superior stability and tolerance to wide range of pH (2–12), temperature (15–45 °C) and co-existing substrate. The reactive oxygen species, which resulted in the catalytic degradation of TZ followed the order of SO 4 ∙− > ∙OH > O 2 ∙− > 1 O 2 , were identified by electron spin resonance and quenching tests. It demonstrated that the radical pathway accomplished with non-radical pathway contributed to the enhanced degradation of TZ, which was further identified by electrochemical experiments. Moreover, the possible degradation pathway of TZ was ascertained and proposed through DFT calculation and LC-MS analysis. These findings illustrated that the novel magnetic biochar would be a promising persulfate catalyst for the treatment of refractory organic matters. In addition, it also provided a new alternative method for the resource utilization of FS and SS.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Zimo Lou,Jiang Xu,Jiasheng Zhou,Kunlun Yang,Zhen Cao,Yizhou Li,Yuanli Liu,Liping Lou,Xinhua Xu
Atomic H* has been regarded as the key active species for the electrocatalytic hydrodechlorination (ECH), and the electrode design and operation conditions are related to the atomic H* generation. However, there is limited understanding of how the operation parameters affect the atomic H* generation and utilization. Due to the fact that Pd was inefficient in water dissociation step, MnO 2 was combined with Pd to construct a novel Pd/MnO 2 /Ni foam cathode. Cyclic voltammetry confirmed that Pd/MnO 2 /Ni foam cathode with MnO 2 load of 0.51 mg cm −2 possessed the highest atomic H* generation and ECH activity. Excessive Pd load (>0.44 mg cm −2 ) was detrimental to ECH because of the side hydrogen evolution reaction (HER). Operation conditions (e.g. applied current and electrolyte concentration) would directly affect the cathode potential, which was an important indicator of the atomic H* generation. The optimal cathode potential was determined to be −0.85 V when the applied current was 10 mA in this study. The electrolyte concentration of 10–15 mM was able to provide sufficient atomic H* for ECH, while excessive input of electrolyte would favor HER but inhibit ECH. ECH at acidic and neutral/alkaline solution underwent different pathways for atomic H* generation and further affect the utilization of atomic H*. After 120 min reaction, >70% of atomic H* could be selectively used for ECH at initial pH of 4.0 and 5.0, while only ∼37% was used for ECH at initial pH of 7.0. This work correlated the reactivity of electrode with the atomic H* and cathode potential, which would provide strategies for ECH catalyst design and operation optimization.
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Nanomaterials
·
2019
·Vol. 9
·期 2
·E210
·
IF 4.034
Qingtong Zhang,Mingfu Li,Chenyan Guo,Zhuan Jia,Guangcong Wan,Shuangfei Wang,Douyong Min
Lignin is the second largest naturally renewable resource and is primarily a by-product of the pulp and paper industry; however, its inefficient use presents a challenge. In this work, Fe₃O₄ nanoparticles loaded on lignin nanoparticles (Fe₃O₄@LNPs) were prepared by the self-assembly method and it possessed an enhanced peroxidase-like activity. Fe₃O₄@LNPs catalyzed the oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) in the presence of H₂O₂ to generate a blue color, was observable by the naked eye. Under the optimal conditions, Fe₃O₄@LNPs showed the ability of sensitive colorimetric detection of H₂O₂within a range of 5⁻100 μM and the limit of detection was 2 μM. The high catalytic activity of Fe₃O₄@LNPs allows its prospective use in a wide variety of applications, including clinical diagnosis, food safety, and environmental monitoring.
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CATALYSIS TODAY
·
2018
·
IF 4.667
Bo Wang,Masakazu Anpo,Jing Lin,Can Yang,Yongfan Zhang,Xinchen Wang
The preparation of ternary hexagonal boron carbon nitride (h-BCN) nanosheets was carried out by doping biomass glucose in situ into hexagonal boron nitride (h-BN). With this method, the construction of a two-dimensional (2D) semiconductor with tunable bandgap and characteristic adsorption ability toward organic molecules was achieved by maintaining the specific structure of h-BN and π-π interactions toward aromatic compounds. The ternary 2D h-BCN nanosheets worked effectively not only as a desirable adsorbent but also as an activator to benzene. Furthermore, the unique 2D h-BCN nanosheets were found to work as effective photocatalysts to convert benzene into phenol with less over-oxidation, leading to the development of a new type of Fenton oxidation reaction as the one-step visible light-driven hydroxylation of benzene. An optimal yield of 14.0% and its selectivity of 88.3% for the photocatalytic production of phenol from benzene were achieved by using h-BCN in the presence of FeCl 3 and H 2 O 2 in sustaining the same reactivity even after 4 cycles. This present study reports the latest development of phenol production from benzene by applying 2D h-BCN nanosheets as an artificial photosynthetic catalyst.
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RSC Advances
·
2014
·Vol. 4
·期 94
·52402-52409
·
IF 3.708
Yong Liu,Lungang Chen,Tiejun Wang,Ying Xu,Qi Zhang,Longlong Ma,Yuhe Liao,Ning Shi
Non-edible cellulose has attracted considerable attention to be converted into valuable platform chemicals. Direct transformation of cellulose to C6 alditols (mannitol and sorbitol) provides a sustainable route. A productive approach is presented in this work using a Ru/C catalyst combined with H+-released boron phosphate in an aqueous phase. A yield of C6 alditols as high as 74.9% with a 91% conversion of cellulose is achieved. By adding silica–alumina materials, the yield of C6 alditols can be improved to 93.5% with complete conversion. The acid sites gradually released from boron phosphate under hydrothermal conditions could promote the hydrolysis of cellulose without significant degradation of glucose. Furthermore, the interaction of boric acid with C6 alditols may form borate–polyol complexes, which can enhance the stability of the C6 alditols to avoid further hydrogenolysis and dehydration of the C6 alditols formed. Due to the adsorption ability of the substrate, the addition of silica–alumina materials with a high content of silica leads to improved performance.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Ying Yang,Xuebo Cao,Lin Huang,Quankun Li,Li Gu,Zheng Yan,Mengli Li,Ruobin Cheng,Zhufeng Lu,Ai-Jun Wang,Wenchao Yang
Electrochemical oxidization of crude ethylene glycol (EG) to fine chemicals driven by sustainable energy is an eco-friendly solution to the upcycling of end-of-life polyethylene terephthalate (PET) wastes. Here, pseudo Ag x -Pt y Pd z core–shell electrocatalyst capable of hybrid oxidation of EG to formate (FA) is designed and synthesized. The trimetallic system consists of Ag nanowire and ultrathin PtPd alloy skin with defects, such as holes and grooves. The defects expose the Ag core to the surroundings and convert Ag 0 to Ag 2+ active species at appropriate potential (> 1.2 V vs RHE). Thus, hybrid EG oxidization reaction is realized on the Ag x -Pt y Pd z electrocatalyst, where PtPd skin catalyzes EG oxidization through conventional Faradaic electrode process owing to inherent activities of Pt and Pd, while Ag 2+ serves as auxiliar oxidant to oxidize EG/intermediates (non-Faradaic reaction). Such a hybrid oxidization strategy reinforces the removal of adsorbates on Ag x -Pt y Pd z electrocatalyst and refresh the active sites timely. Eventually, ultrahigh specific activity (24.45 A mg −1 PtPd ) and long-term stability (> 3000 h at current density ≥ 400 mA cm −2 ) are delivered by the system. The finding of Ag 2+ -enhanced alcohol oxidization reactions introduces a new paradigm for designing high-performance electrocatalysts for energy and environmental applications.
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Nanomaterials
·
2024
·Vol. 14
·期 20
·1629
·
IF 4.4
Penghui Lei,Qing Chang,Mingkun Xiao,Chao Ye,Pan Qi,Fangjie Shi,Yuhua Hang,Qianwu Li,Qing Peng
A new type of SiCf/TiC-Ti3SiC2composite was prepared by the Spark Plasma Sintering (SPS) method in this work. The phase transformation and interface cracking of this composite under ion irradiation (single Xe, Xe + He, and Xe + He + H ions) and subsequent annealing were analyzed using transmission electron microscopy (TEM), mainly focusing on the interface regions. Xe ion irradiation resulted in the formation of high-density stacking faults in the TiC coatings and the complete amorphization of SiC fibers. The implanted H ions exacerbated interface coarsening. After annealing at 900 °C for 2 h, the interface in the Xe + He + H ion-irradiated samples was seriously damaged, resulting in the formation of large bubbles and cracks. This damage occurred because the H atoms reduced the surface free energy, thereby promoting the nucleation and growth of bubbles. Due to the absorption effect of the SiCf/TiC interface on defects, the SiC fiber areas near the interface recovered back to the initial nano-polycrystalline structure after annealing.
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