Journal of Energy Chemistry
·
2023
·
IF 13.1
Mengxia Li,Tianxi Zheng,Dongfei Lu,Shiwei Dai,Xin Chen,Xinchen Pan,Dibo Dong,Rengui Weng,Gang Xu,Fanan Wang
The electrochemical hydrogenation of HMF to BHMF is an elegant alternative to the conventional thermocatalytic route for the production of high-value-added chemicals from biomass resources. In virtue of the wide potential window with promising Faradic efficiency (FE) towards BHMF, Cu-based electrode has been in the center of investigation. However, its structure–activity relationship remains ambiguous and its intrinsic catalytic activity is still unsatisfactory. In this work, we develop a two-step oxidation–reduction strategy to reconstruct the surface atom arrangement of the Cu foam (CF). By combination of multiple quasi-situ/in-situ techniques and density functional theory (DFT) calculation, the critical factor that governs the reaction is demonstrated to be facet effect of the metallic Cu crystal: Cu(110) facet accounts for the most favorable surface with enhanced chemisorption with reactants and selective production of BHMF, while Cu(100) facet might trigger the accumulation of the by-product 5,5′-bis(hydroxymethy)hydrofurion (BHH). With the optimized composition of the facets on the reconstructed Cu(OH) 2 -ER/CF, the performance could be noticeably enhanced with a BHMF FE of 92.3% and HMF conversion of 98.5% at a potential of −0.15 V versus reversible hydrogen electrode (vs. RHE) in 0.1 M KOH solution. This work sheds light on the incomplete mechanistic puzzle for Cu-catalyzed electrochemical hydrogenation of HMF to BHMF, and provides a theoretical foundation for further precise design of highly efficient catalytic electrodes.
研究领域:
化学工程
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催化科学
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材料科学
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产品关联
DOI
高影响因子
Chem Catalysis
·
2023
·
IF 9.4
Zhongliang Huang,Siyuan Hu,Yinan Xu,Jinxin He,Dongren Cai,Kang Sun,Jianchun Jiang,Guowu Zhan
Summary The interfacial sites of metal-support catalysts are crucial for catalytic reactions. Herein, we designed well-defined N-Co 3 O 4 /Pt catalysts with N-tailoring metal-support interfaces to promote catalytic activity toward CO oxidation under humid environments. A series of N-Co 3 O 4 /Pt catalysts were fabricated using ZIF-67 nanocubes as self-sacrificing templates, which showed exceptionally high catalytic activity in low-temperature CO oxidation. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study indicates that H 2 O molecules undergo dissociative adsorption to form active –OH species (Co 3+ –OH–Pt). Isotopic labeling technique indicates that H 2 O molecules (or –OH groups) contribute to ∼65% of CO 2 production in CO oxidation. Moreover, the amount of N dopant that stabilized the Co 3+ –OH–Pt species was highly dependent on the H 2 O-soaking conditions of ZIF-67/Pt. Density functional theory (DFT) calculations suggest that the COOH ∗ pathway of CO oxidation over the N-Co 3 O 4 /Pt interface is energetically favorable in humid conditions. In particular, the N doping could stabilize the Co 3+ –OH–Pt interface and simultaneously reduce the energy barrier of CO 2 formation from COOH ∗ intermediates.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
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2022
·
IF 9.463
Haimo Zhang,Jun Zhong,Huilong Xu,Xuanyu Shi,Li Yang,Shihao Sun,Yihu Song,Min Zuo,Qiang Zheng
Bicontinuous structured nanocomposites with nanoparticles (NPs) assembled at the interface between two fluids have a wealth of proposed applications. Here, we used a universal and facile strategy to prepare such various bicontinuous stable nanocomposites filled with homopolymer-brush grafted NPs of various dimensions. We investigated the detailed formation of such nanocomposites online and proposed a model to fit and predict the effect of NPs at the interface on the domain coarsening of blend matrix and further stabilizing their bicontinuous morphology, based on the influence of NPs percolation on the time-dependent effective interfacial tension. The morphology evolution of nanocomposites can be predicted from the volume fraction of NPs, annealing time and temperature, which may provide some guidelines for the design and preparation of bicontinuous structured nanocomposites with the controllable and stable structure.
研究领域:
材料科学
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纳米技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Min Yang,Xiaohua Ren,Leixin Hu,Weilin Guo,Jinhua Zhan
Advanced oxidation processes (AOPs) based on the activation of persulfate (PS) by minerals have been widely used in environmental remediation. Herein, two goethite materials with different contents of exposed {0 2 1} facet were synthesized and used as the catalysts for PS activation to degrade tetracycline. Results showed that exposed facets significantly affected their catalytic activity. Goethite exposed with more {0 2 1} facet exhibited better catalytic performance. Attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), and electrochemical analysis suggested that the surface Fe(II)/Fe(III) redox cycle, the abundant surface hydroxyl density and the easier generation of active radicals by activating PS were responsible for the excellent catalytic performance of goethite with more {0 2 1} facet exposed. Furthermore, the density functional theory (DFT) calculations further confirmed that {0 2 1} facet was more favorable for the activation of PS than {1 1 0} facet. The electron paramagnetic resonance (EPR) and radical scavenging experiments indicated that both sulfate radicals and hydroxyl radicals participated in the degradation process. This study provides new insights into the PS heterogeneous activation by facet-dependent goethite in environmental catalysis.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Sibo Chen,Zhi Yang,Jiadong Chen,Jihai Liao,Siyuan Yang,Feng Peng,Liang-Xin Ding,Guangxing Yang,Shengsen Zhang,Yueping Fang
Heterogeneous nano-metal structures are widely used in the field of photocatalysis as an efficient cocatalyst, but the structure–activity relationship has not been elucidated clearly. In this work, a classical CuCo@C nanoparticle with a core of bimetallic CuCo and a carbon shell was used as a cocatalyst to explore and reveal the mechanism of interfacial effect for enhanced photocatalytic hydrogen evolution . It was found that the bimetallic CuCo had a heterogeneous structure with abundant Cu-Co interfaces. The desirable visible-light-driven photocatalytic hydrogen evolution rate of CuCo@C/g-C 3 N 4 was much higher than that of Cu@C/g-C 3 N 4 , Co@C/g-C 3 N 4 , and superior to that of the control group loaded with 1 wt% Pt (Pt/g-C 3 N 4 ). According to the experimental characterizations and density functional theory calculations, electrons were enriched at the Cu-Co interface, which can promote the electron-hole pairs separation and accelerate charge transfer of the g-C 3 N 4 host photocatalysts. On the other hand, the surface carbon layer and Cu-Co interface modulated the H adsorption free energy on the CuCo@C, which was favorable for hydrogen evolution. It is conceivable that further investigating and tuning different metal interfaces will facilitate the large-scale application of bimetallic cocatalysts.
研究领域:
材料科学
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光催化
✓ 已验证
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2024
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IF 5.1
Shuai Nie,Jing Li,Yunxia He,Xitao Yin
Gas sensors with the p–n heterojunction have demonstrated distinct sensing responses to reducing gases, yet a clear understanding of the reaction pathways and selective adsorption mechanisms for specific gas components remains elusive, impeding practical applications. In this study, we constructed an atomic-level NiO–In 2 O 3 heterojunction and explored its adsorption behaviors and sensing properties for CO and H 2 by first-principles calculations. Analysis of its electronic properties, focusing on binding energy, differential charge density, and density of states, confirmed the creation of a highly stable NiO–In 2 O 3 heterojunction and alterations in the coordination environment of the surface-active atoms. These changes potentially led to differences in the affinity between the gas molecules and the adsorption sites. The calculations of the adsorption properties revealed that the adsorption capacity of H 2 is relatively weak compared to the strong interactions between CO and heterojunction surface atoms, indicating a readily variable reaction pathway for H 2 . Consequently, the adsorption configuration at the interface site on the NiO–In 2 O 3 heterojunction surface exhibited a predominantly p-type response for CO and a unique n-type response for H 2 . This interfacial effect of the heterojunction is crucial for the selective adsorption of CO and H 2 . Furthermore, the opposite response signal was verified by gas sensing tests, which also presented the superior stability of the NiO–In 2 O 3 sensor. The p–n heterojunction of the corresponding composites was effectively characterized. This research offers new insights into the selective adsorption mechanism, paving the way for the development of gas sensors.
研究领域:
材料科学
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传感器技术
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Qing Ji,Weiheng Chen,Xiaoping Chen,Xiaoyan Wang,Qingyu Dong,Shanshan Yin,Yanbin Shen,Peter Müller-Buschbaum,Ya-Jun Cheng,Yonggao Xia
Niobium pentoxides (Nb2O5) present great potential as next-generation anode candidates due to exceptional lithium-ion intercalation kinetics, considerably high capacity, and reasonable redox potential. Although four phases of Nb2O5 including hexagonal, orthorhombic, tetragonal, and monoclinic polymorphs show diverse characteristics in electrochemical performance, stable lifetime, high specific capacity, and fast intercalation properties cannot be delivered simultaneously with a single phase. Herein, this issue is addressed by generating a homogeneous mixture of orthorhombic and monoclinic crystals at the nanoscale. Reversible lithium-ion intercalation/deintercalation of the monoclinic phase is achieved, and exceptional lithium storage sites are created at the interface of the two phases. As a result, electrochemical features of stable lifetime from the orthorhombic phase and high specific performance from the monoclinic phase are harmoniously combined. This dual-phase Nb2O5/C nanohybrids deliver as high as 380 mA h g–1 (0.01–3.0 V) and 184 mA h g–1 (1.0–3.0 V) after 200 cycles. The essential principle of property enhancement is further confirmed through in situ XRD measurements and DFT calculations. The dual-phase concept can be further applied on electrodes with multiphases to achieve high electrochemical performance.
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemSusChem
·
2018
·Vol. 11
·期 22
·3965-3974
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IF 7.411
Hai Wang,Liang Wang,Jian Zhang,Chengtao Wang,Ziyu Liu,Xinhua Gao,Xiangju Meng,Seung Jo Yoo,Jin-Gyu Kim,Wei Zhang,Feng-Shou Xiao
Graphical Ready layer one : A newly synthesized catalyst with layered cobalt oxide on the surface of titania (layer-CoO x /TiO 2 ) is highly selective towards the aerobic oxidation of C−H bonds in a series of hydrocarbons. In-depth structural and functional characterization reveal that the layer-CoO x /TiO 2 readily reacts with O 2 for the adsorption and activation of C−H bonds. Construction of efficient interfaces to improve the performance of supported metal catalysts is a challenging but effective technique. A newly synthesized catalyst with layered cobalt oxide on the surface of titania (layer-CoO x /TiO 2 ) is highly selective towards the aerobic oxidation of C−H bonds in a series of hydrocarbons under sustainable conditions. The layer-CoO x /TiO 2 easily outperforms the state-of-the-art noble metal catalysts and homogeneous cobalt salts used in industry. In-depth structural and functional characterization reveal that the layer-CoO x /TiO 2 readily reacts with O 2 for the adsorption and activation of C−H bonds. The layered structure of CoO x can maximize the interfacial effect of CoO x /TiO 2 leading to a good performance for the oxidation of C−H bonds.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
Chemical Science
·
2019
·Vol. 10
·期 12
·3556-3566
·
IF 9.556
Yanan Liu,Alan J. McCue,Pengfei Yang,Yufei He,Lirong Zheng,Xingzhong Cao,Yi Man,Junting Feng,James A. Anderson,Dianqing Li
The impregnation method is commonly employed to prepare supported multi-metallic catalysts but it is often difficult to achieve homogeneous and stable alloy structures. In this work, we revealed the dependence of alloying behavior on the support morphology by fabricating Ni–Cu over different shaped CeO2. Specifically, nanocube ceria favoured the formation of monometallic Cu and Ni-rich phases whereas polycrystalline and nanorod ceria induced the formation of a mixture of Cu-rich alloys with monometallic Ni. Surprisingly, nanopolyhedron (NP) ceria led to the generation of homogeneous Ni–Cu nanoalloys owing to the equivalent interactions of Ni and Cu species with CeO2 (111) facets which exposed relatively few coordinative unsaturated sites. More importantly, a strong interfacial effect was observed for Ni–Cu/CeO2-NP due to the presence of CeOx adjacent to metal sites at the interface, resulting in excellent stability of the alloy structure. With the aid of CeOx, NiCu nanoalloys showed outstanding catalytic behaviour in acetylene and hexyne hydrogenation reactions. This study provides valuable insights into how fully alloyed and stable catalysts may be prepared by tailoring the support morphology while still employing a universal impregnation method.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 14
·8332-8339
·
IF 3.119
Pinhua Zhang,Hongyang Zhu,Kaifeng Xue,Li Chen,Changmin Shi,Dongchao Wang,Jianfu Li,Xiaoli Wang,Guangliang Cui
2D heterostructures are promising gas sensor materials due to their surface/interface effects and hybrid properties. In this research, Cu2O/Fe2O3 heterostructure ordered arrays were synthesized using an in situ electrodeposition method for H2S detection at low temperatures. These arrays possess a periodic long range ordered structure with horizontal multi-heterointerfaces, leading to superior gas sensitivity for synergistic effects at the heterointerfaces. The sensor based on the Cu2O/Fe2O3 heterostructure ordered arrays exhibits a dramatic improvement in H2S detection at low temperatures (even as low as −15 °C). The response is particularly significant at room and human body temperatures since the conductivity of the arrays can change by up to three orders of magnitude in a 10 ppm H2S atmosphere. These good performances are also attributed to the formation of metallic Cu2S conducting channels. Our results imply that the Cu2O/Fe2O3 heterostructure ordered arrays are promising candidates for high-performance H2S gas sensors that function at low temperatures as well as breath analysis systems for disease diagnosis.
研究领域:
材料科学
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传感器技术
·
气体检测
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED ENGINEERING MATERIALS
·
2016
·Vol. 19
·期 2
·1600601
·
IF 1.817
Haiquan Zhang,Yanping Yuan,Qinrong Sun,Xiaoling Cao
Development of a polyethylene glycol (PEG) phase change material (PCM) is a popular research topic. Chemical reactions between the PEG and additive degrade the energy storage density obviously. We prepare a PEG8000/copper-based oxide composite to solve this problem. FT-IR results show that the molecular structure of the PEG8000 polymer does not change, thereby, indicating that no chemical reactions occur. Crystallization temperature of the composite is increased by 4.8 °C, corresponding to the formation of the hydrogen bond during the exothermic process. Crystallization fraction (Fc) of the composites is over 100% on the role of the interface effect. The present study represents an important step toward the development of composite PCMs with highly comprehensive performance.
研究领域:
材料科学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2012
·
IF 0.901
Fang WANG,Chenglu LIU,Zhiqiang ZHOU,Peiyun JIA,Jun LIN
YVO 4 :Eu nanocrystalline phosphors were successfully prepared at 400 °C in equal moles of NaNO 3 and KNO 3 molten salts. NaOH concentration and annealing temperature played important roles in phase purity and crystallinity of the nanocrystallines, and the optimum NaOH concentration and annealing temperature were 6:40 and 400 °C, respectively. The nanocrystallines were well crystallized with a cubic morphology in an average grain size of 18 nm. Upon excitation of the vanadate groups at 314 nm, YVO 4 :Eu nanocrystallines exhibited the characteristic emission of Eu 3+ , which indicated that there was an energy transfer from vanadate groups to Eu 3+ . Moreover, the influence of superficial effect, especially the dangling bonds on the structure and luminescent properties of the nanocrystallines was discussed in detail.
研究领域:
材料科学
·
光学
✓ 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）