AICHE JOURNAL
·
2025
·
IF 4
Ziqi Bian,Minhao Chen,Xiaohu Ge,Ningchao Zhu,Yueqiang Cao,Hao Jiang,Jing Zhang,Gang Qian,Xinggui Zhou,Xuezhi Duan
Designing and fabricating uniformly dispersed non-precious metal active sites with tuned geometric configurations and local coordination environments for the selective conversion of functional groups to desired products is of great importance but remains challenging in industrial catalytic processes. In this work, we propose a straightforward method for synthesizing the Co 3 Sn 2 intermetallic catalyst through the structural conversion of layered double hydroxide precursors, thereby constructing suitable Sn-modified Co active sites and an optimized catalytic environment for propyne semihydrogenation. Characterizations using x-ray diffraction, high-resolution transmission electron microscopy, and x-ray absorption spectroscopy characterizations are combined to identify the formation of P6 3 /mmc Co 3 Sn 2 intermetallic phase. Catalytic performance tests show that the Co 3 Sn 2 catalyst achieves 95.0% propylene selectivity with nearly complete propyne conversion. Temperature-programmed surface reaction and desorption measurements combined with theoretical calculations demonstrate that the good selectivity is driven by the facile desorption of propylene from Sn-modified Co sites rather than its further hydrogenation.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nano Materials Science
·
2021
·
IF 0
Ning You,Shuai Cao,Mengqiu Huang,Xiaoming Fan,Kun Shi,Haijian Huang,Zhangxian Chen,Zeheng Yang,Weixin Zhang
Improving catalytic activity and durabilty through the structural and compositional development of bifunctional electrocatalysts with low cost, high activity and stability is a challenging issue in electrochemical water splitting. Herein, we report the fabrication of heterostructured P-CoMoO 4 @NiCoP on a Ni foam substrate through interface engineering, by adjusting its composition and architecture. Benefitting from the tailored electronic structure and exposed active sites, the heterostructured P-CoMoO 4 @NiCoP/NF arrays can be coordinated to boost the overall water splitting. In addition, the superhydrophilic and superaerophobic properties of P-CoMoO 4 @NiCoP/NF make it conducive to water dissociation and bubble separation in the electrocatalytic process. The heterostructured P-CoMoO 4 @NiCoP/NF exhibits excellent bifunctional electrocatalysis activity with a low overpotential of 66 mV at 10 mA cm −2 for HER and 252 mV at 100 mA cm −2 for OER. Only 1.62 V potential is required to deliver 20 mA cm −2 in a two-electrode electrolysis system, providing a decent overall water splitting performance. The rational construction of the heterostructure makes it possible to regulate the electronic structures and active sites of the electrocatalysts to promote their catalytic activity.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 25
·14451-14458
·
IF 12.732
Yonggang Liu,Haijing Li,Junfu Li,Xiaoshuang Ma,Zhiming Cui,Daqiang Gao,Zhenghua Tang
Two-dimensional (2D) rhenium disulfide (ReS2) has been attracting immense interest as a highly promising hydrogen evolution reaction (HER) electrocatalyst recently. However, the HER catalytic active sites of ReS2 are still limited to the finite edges of the nanosheets and the basal-plane is catalytically inert. How to activate the in-plane catalytic activity of ReS2 accordingly becomes the sticking point to further boost its H2 evolution efficiency. Here, the fluorinated ReS2 hierarchical structure assembled as ultrathin nanosheets is proved to exhibit excellent HER activity, where the optimal sample of ReS2-F5.93 shows a low overpotential of 142 mV vs. RHE at a current density of 10 mA cm−2, a Tafel slope of 64 mV dec−1, and significantly improved stability. The enhanced HER performance is mainly attributed to the synergistic effects of increased in-plane active sites and remarkably accelerated charge transfer kinetics. The density functional theory calculation results reveal that F doping can yield the optimal H* adsorption Gibbs free energy and meanwhile increase the electronic states near the Fermi level for accelerated electron transfer. This work can broaden the horizon for designing efficient HER electrocatalysts via activating the in-plane catalytic activity of transition metal dichalcogenides (TMDs).
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Jing Cao,An Li,Yicen Zhang,Linchao Mu,Xi Huang,Yankun Li,Tao Yang,Cen Zhang,Congshan Zhou
To prepare catalyst with high activity, high selectivity and good stability remains the biggest challenge in the hydrodeoxygenation (HDO) of phenols by adopting MoS 2 -based sulfides as catalysts. Herein, we report a simple hydrothermal method to synthesize highly-dispersed nano-MoS 2 with abundant defects and some curved slabs. All these advantages enable nano-MoS 2 to provide a large number of coordination unsaturated sites to anchor Co atoms. The unsupported Co-doped catalyst with an optimal Co/(Co + Mo) molar ratio of 0.3 exhibited excellent performance in the HDO of p -cresol with conversion of 98.7 % and toluene selectivity of 98.9 % at 220 °C. Moreover, the optimized Co/MoS 2 -0.3 catalyst had a good stability after reaction of 72 h. The excellent HDO performance was attributed to the formation of abundant Co-Mo-S active sites which optimize the electrical structure of nano-MoS 2 by Co promoter.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Ke Li,Hao Fang,Xiuzhi Duan,Dongshun Deng
Development of high-efficient solvents for NH 3 capture to improve the quality of atmosphere and ecological environment is a hot research topic. Deep eutectic solvents (DESs) as NH 3 absorbents can overcome some problems troubling the traditional NH 3 capture process. In this work, NH 4 SCN was paired with imidazole (Im) DESs to form low viscous DESs with dual active sites for highly efficient NH 3 absorption. The effects of absorption temperature, gas flow rate, water content, molar ratio on NH 3 absorption performance as well as physical properties of NH 4 SCN/Im DESs were systematically investigated. The results show that NH 4 SCN/Im DESs can rapidly capture NH 3 with good recycling performance, while the gas flow rate only shortens the absorption time. The NH 3 absorption capacity of NH 4 SCN/Im DESs decreased with increasing temperature and NH 4 SCN/Im molar ratio. The absorption capacity of NH 4 SCN/Im (1:2) DES reaches 9.65 mol NH 3 /kg DESs for atmospheric NH 3 . Based on 1 H NMR and IR spectroscopy analysis, the strong hydrogen bond between protic ammonium cation and NH 3 plays the major essence of efficient NH 3 capture for NH 4 SCN/Im DESs.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Dashi Lei,Juanqin Xue,Xiangyu Peng,Shuhao Li,Qiang Bi,Changbin Tang,Liang Zhang,Jing Zhang
Inorganic arsenic threatens human health due to its high mobility and toxicity. In this work, rapid and effective treatment of As(III) wastewater was achieved by Z-Scheme photocatalyst (ZnFe 2 O 4 /Ag/AgCl). By means of peroxymonosulfate (PMS) activation, 50 mg/L As(III) was completely removed within 20 min under light irradiation. During photocatalytic system, free radicals ( SO 4 − , OH, O 2 − ) and non-radicals ( 1 O 2 ) were responsible for As(III) removal. The fast PMS activation was attributed to the loop conversion of Fe(III)/Fe(II) and Ag 0 /Ag + . Besides, density functional theory (DFT) calculations exhibited that Fe atoms were active sites for As(III) adsorption and Ag nanoparticles were spots for PMS activation. Specially, the dual active sites on photocatalyst could effectively minimize the distance between oxidizing product with arsenite molecular and thus facilitate As(III) fast oxidation.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yingni Yu,Jing Liu,Yingju Yang,Junyan Ding,Aijia Zhang
Iron oxide (Fe 2 O 3 ) has been used as an effective sorbent to remove various heavy metals due to its large adsorption capacity and low cost. The cadmium capture capability of Fe 2 O 3 sorbent was investigated in the simulated flue gas at the temperatures of 700–1100 °C. Fe 2 O 3 sorbent exhibited much better Cd adsorption capability than SiO 2 and Al 2 O 3 sorbents. The largest Cd adsorption capacity of Fe 2 O 3 sorbent was 86.7 mg/g at 700 °C. The XPS analysis demonstrated that Fe 3+ might partially participate in the cadmium adsorption process. A large quantity of CdO was generated and adsorbed on the Fe 2 O 3 surface. The density functional theory (DFT) calculations were used to determine the active sites and the involved mechanism of different cadmium species adsorption over Fe 2 O 3 sorbent. Cd, CdCl 2 , and CdO can be stably adsorbed on the Fe 2 O 3 surface with the adsorption energies of −40.64 kJ/mol, −237.42 kJ/mol, and −375.03 kJ/mol, respectively. The results illustrate that the Fe atoms are the essential active sites for cadmium species adsorption on Fe 2 O 3 surface. The orbital hybridization between cadmium atom and Fe site suggests that the strong interaction occurs during Cd adsorption process. Both physisorption and chemisorption mechanisms were responsible for the cadmium capture by Fe 2 O 3 sorbent.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Xuliang Pang,Huaiquan Zhao,Yifei Huang,Youchao Liu,Hongye Bai,Weiqiang Fan,Weidong Shi
Achievement of the intrinsic activity by in situ electrochemical reconstruction has been becoming a great challenge for designing a catalyst. Herein, an effective electrochemical strategy is proposed to reconstruct the surface of the CF–CuO/CeO2 precursor. Under the stimulation of oxidative/reductive potential, abundant active sites were successfully generated on the surface of CF–CuO/CeO2. Remarkably, the implantation of oxygen vacancy-rich CeO2 synergistically optimizes the chemical composition and electronic structure of CF–CuO/CeO2, greatly promoting the generation of active species. Systematic electrochemical experiments indicate that the superior catalytic performance of reconstructed CF–CuO/CeO2 could be attributed to CuOOH/CeO2 and Cu2O/Ce2O3 active species, respectively. The oxidative-/reductive-activated CF–CuO/CeO2 was further employed in a paired cell for the synergistic catalysis of hydroxymethylfurfural oxidation with 4-nitrophenol hydrogenation. As a result, nearly 100% Faraday efficiency for furandicarboxylic acid/4-aminophenol production was achieved in the paired system (−0.9 V vs Ag/AgCl, 1.5 h). Therefore, the electrochemical reconstruction via oxidative/reductive activation has been confirmed as a feasible approach to significantly excite the intrinsic activity of a catalyst.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Cheng Liu,Yao Qin,Wei Guo,Yingzhang Shi,Zhiwen Wang,Yan Yu,Ling Wu
Enormous efforts have been devoted to exploring the influence of the materials’ morphology on photocatalytic performance, while the role of active site between them attracts less attention. Herein, three types of anatase nano-TiO 2 with different morphologies were successfully prepared for visible-light-driven photocatalytic selective oxidation of benzylamine. The material properties of the samples were systematically studied by various characterization techniques such as XRD, SEM, TEM, AFM, XPS, UV–vis DRS, ESR and in situ FTIR. Due to possessing clear advantages especially for having more active sites (coordinatively unsaturated Ti atoms and oxygen vacancies), the TiO 2 with porous structure shows more excellent photocatalytic performance than the other samples. Coordinatively unsaturated Ti atoms can chemisorb and activate benzylamine molecules via forming H-N … Ti coordination species, whose absorption property of visible light guarantees that TiO 2 samples can achieve the photocatalytic process under visible light. Oxygen vacancies can chemisorb and activate oxygen molecules to form reactive oxygen species (superoxide radical) by the reduction of photogenerated electrons. Finally, a possible synergetic mechanism based on the interaction of reactants and catalyst interfaces was proposed at the molecular level to illustrate the photocatalytic process.
研究领域:
材料科学
·
光催化
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Ruiqi Guo,Jialun Shi,Lan Hong,Kaiwen Ma,Wenxiang Zhu,Haiwei Yang,Jiajie Wang,Huihua Wang,Minqi Sheng
Electrocatalytic water splitting is a desirable and sustainable strategy for hydrogen production yet still faces challenges due to the sluggish kinetics and rapid deactivation of catalysts in the oxygen evolution process. Herein, we utilized the metal-catalyzed growth technology and phosphating process to fabricate self-supported electrodes (CoxPy@CNT-CC) composed of carbon nanotube (CNT) arrays grown on carbon cloth (CC); thereinto, cobalt-based phosphide nanoparticles (CoxPy) are uniformly encapsulated in the cavity of the CNTs. After further optimization, when the nanoparticles are in the composite phase (CoP2/Co2P), CoP2/Co2P@CNT-CC served as catalytic electrodes with the highest activity and stability for electrocatalytic water splitting in an alkaline medium (1.0 M KOH). The as-prepared CoP2/Co2P@CNT-CC integrates the advantages of the abundant active sites and confinement effect of CNTs, imparting promising electrocatalytic activities and stability in catalyzing both hydrogen evolution reaction and oxygen evolution reaction. Remarkably, electrocatalytic water splitting cells assembled using CoP2/Co2P@CNT-CC electrodes as the cathode and anode, respectively, require a cell voltage of 1.55 V at 10 mA cm–2, which is lower than that of the commercially noble Pt/C/CC and RuO2/CC catalyst couple (1.68 V). Besides, a CoP2/Co2P@CNT-CC||CoP2/Co2P@CNT-CC system shows outstanding durability for a period of 100 h at 10 mA cm–2. This work may provide new ideas for designing bifunctional electrocatalysts for applications in electrocatalytic water splitting.
研究领域:
材料科学
·
电化学
·
能源转换与储存
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CRYSTAL GROWTH & DESIGN
·
2023
·
IF 3.8
Xunming Su,Zhong-Pan Hu,Jingfeng Han,Yingxu Wei,Zhongmin Liu
Developing highly efficient methods to selectively incorporate active metal sites into the zeolite framework is crucial for the large-scale utilization of metal-zeolites in various catalytic reactions including alkane conversion. Herein, ferrous gluconate is developed as an efficient metal precursor to embed Fe atoms into the MFI siliceous zeolite framework. The crystallization time and Si/Fe ratio are systematically investigated. It is revealed that the ferrous gluconate is well soluble and stable under alkaline conditions, allowing ferrous gluconate to participate in the whole crystallization course of zeolite. Multiple characterizations demonstrate that the tetrahedrally coordinated Fe atoms are selectively incorporated into the MFI siliceous zeolite framework (Fe-MFI). A catalytic test in propane dehydrogenation shows that the optimized Fe-MFI zeolite possesses high activity, propylene selectivity, and durability. This study opens an efficient strategy to incorporate isolated Fe atoms into the zeolite framework.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Yanqing Shi,Cai Guo,Huajing Zhou,Liang He,Shaoyun Shan,Tianding Hu
Rational modulation of the local electron density of Cu active site is the key to improve the efficient transfer hydrogenation (CTH) of furfural (FF) on the surface of catalysts with low Cu-loadings. In this paper, a CuMgAl/LSC catalyst with lower Cu content (<3.5 % wt ) was prepared by using porous biochar as a carrier and exploiting the local dispersion and electron-modulation effects of structural elements of hydrotalcite laminates. CTH experiments showed that the conversion of FF and the selectivity of FA could reach more than 99.0 % in isopropanol solution at 170 °C and within 1 h. Catalyst characterization and density functional theory (DFT) calculations demonstrated that the Cu(I) species was the main active site during the CTH process of FF. Doping laminate metals (i.e., Mg, Al) can not only form electron-rich centers by local electron modulation of the active site through the coordination structure of Cu-O-M, lowering its D-band center and achieving higher catalytic activity; Due to the Jahn-Teller effect, the local spatial misalignment of Cu sites formed, which can reduce the risk of over-hydrogenation and improve the FA selectivity. In addition, it can be also found that the Coulomb tractive force of reactive intermediates can lead to the crystal surface reconstruction and structure deterioration of Cu species. The new discovery of the deactivation mechanism can provide a reference for the future design of copper-based catalysts in CTH process of FF.
研究领域:
催化化学
·
材料科学
✓ 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）