Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 8
·4744-4750
·
IF 12.732
Shengqi Wang,Songliang Liu,Ziqiang Wang,Zechuan Dai,Hongjie Yu,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Mesoporous noble metal-based nanoarchitectures with large cavities and accessible active surfaces have been demonstrated as effective catalysts in electrocatalysis fields, but mesoporous rhodium nanotubes have hardly been reported due to the difficulty in regulating the discrepancy between the reduction rate and micelle assembly rate. Herein, we present a simple dual-template strategy for in situ fabrication of one-dimensional rhodium mesoporous nanotubes (Rh MNTs), in which the obtained Ni nanowires and diblock copolymer micelles facilitate the evolution of tubular interiors and mesoporous exteriors, respectively. The well-developed hollow mesoporous structure can not only provide sufficient active centers and facilitated channels, but can also prevent catalyst aggregation. Therefore, the generated Rh MNTs exhibit excellent activity, favorable kinetics and high durability for the methanol oxidation reaction, which are superior to those of traditional commercial Pt black. This work sheds light on the fabrication of one-dimensional metallic mesoporous nanotube structures for extensive electrocatalytic applications.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2024
·
IF 4.3
Xu-hong Han,Xue-wei Zhao,Kun Huang,Lei Yang,Qing Wang,Peng-fei Shi
Tracing copper ions levels in the environment and subcellular microenvironment is crucial due to the key role copper ions play in physiological and pathological processes. Herein, a novel naphthalimide-fused rhodamine probe Rh-Naph-Cu was prepared through modification with phenylhydrazine to produce a closed and non-fluorescent spirolactam. Based on the copper-induced spirolactam ring-opening and hydrolysis process, Rh-Naph-Cu can be employed as a fluorescence off–on probe for copper ions with high selectivity, high sensitivity (limit of detection: 33.0 nM), broad pH-response range (pH: 5.0–10.0), and color change visible with the naked eye. Rh-Nap-Cu could be made into test strips for the in-situ chromogenic detection of Cu 2+ . Significantly, Rh-Naph-Cu can be utilized for the detection of copper ions in living HeLa cells and zebrafish, and exhibits excellent lysosomal-targeting ability with high Pearson’s correlation coefficient (PCC) of 0.96.
研究领域:
生物化学
·
分子生物学
·
环境科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 28
·期 55
·e202201430
·
IF 5.02
Yuanyuan Zhang,Jian Liu
Graphical An artificial photosystem was constructed through the covalent attachment of Rh complex onto PCN. The integrated photocatalyst could regenerate NADH efficiently by integrating the light harvesting unit and the electron transfer unit through conjugated connection. By further coupling with FDH immobilized on the hydrophobic membrane, an enhanced HCOOH production could be obtained. Natural photosynthesis is a highly unified biocatalytic system, which coupled cofactor (NAD(P)H) regeneration and enzymatic CO 2 reduction efficiently for solar energy conversion. Mimicking nature, a novel system with Rh complex covalently grafted onto NH 2 -functionalized polymeric carbon nitride (NH 2 -PCN) was constructed. The integrated connection of the light-harvesting and electron mediation modules as Rh m3 -N-PCN could promote the efficient NAD + reduction to NADH. As a result, the integrated system exhibited a conversion of ∼66 % within 20 minutes. By further coupling in situ generated NADH with formate dehydrogenase (FDH), a photoenzymatic production of formic acid (HCOOH) from CO 2 was accomplished. Moreover, by immobilizing FDH onto a hydrophobic membrane, an enhanced HCOOH production of ∼5.0 mM can be obtained due to the concentrated CO 2 on the gas-liquid-solid three-phase interface. Our work herein provides an integrated strategy for coupling the anchored electron mediator with immobilized enzyme for enhanced artificial photosynthesis.
研究领域:
生物化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
REVIEWS ON ADVANCED MATERIALS SCIENCE
·
2022
·Vol. 61
·期 1
·138-145
·
IF 5.028
Yong Guo,Minghu Nie,Yingjie Wang,Zhen Zhong,Yunfeng Liu
Adsorbent is an important waste water-based drilling fluid treatment agent, which can adsorb and settle heavy metal ions, high polymer organics, and other soluble harmful substances in the waste drilling fluid. Traditional adsorbents such as polyaluminum chloride and polyacrylamide will produce other metal ions or toxic monomers after hydrolysis, which cannot fully meet the requirements of safety and environmental protection. Therefore, a new environmentally friendly waste water-based drilling fluid adsorbent, named RH-β-CD, was prepared by the Wilson etherification reaction, which was initiated by epichlorohydrin and ceric ammonium nitrate, and successfully grafted rhamnolipid and amine strong adsorption groups onto β-cyclodextrin. The adsorption effect and environmental protection performance of RH-β-CD on the organic matter and chromium ion in waste sulfonated water-based drilling fluid were evaluated and compared with commonly used adsorbents such as activated carbon, PAM, and polyaluminum chloride. The results show that RH-β-CD can effectively adsorb the organic matter in the filtrate of waste water-based drilling fluids, reduce its chemical oxygen consumption, and reduce the concentration of heavy metal ions in the filtrate. The effect is better than PAM, activated carbon, and polyaluminum chloride, with the BOD 5 /COD cr >20% and EC 50 >1,000,000 mg·L −1 , which is environmentally friendly.
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
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 45
·21560-21567
·
IF 3.925
Jinyang Liu,Yan Zhou,Xiuniang Tan,Shengjiang Zhang,Chunjiao Mo,Xiaobo Hong,Taolong Wu,Xuecai Tan,Yanjuan Liao,Zaiyin Huang
The establishment of heterojunctions is an effective way to improve the performance of semiconductor photocatalysts as a solution to solve environmental pollution problems; however, the decomposition efficiency of organic pollutants driven by sunlight remains a challenge. Herein, CoS2-decorated CdS hetero-junctions as highly efficient photocatalysts were rationally synthesized via a three-step process and CoS2-decorated CdS composites were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, UV-Vis diffusion reflectance spectrometry, fluorescence spectroscopy analysis, X-ray photoelectron spectroscopy, electron paramagnetic resonance spectroscopy, and transient photocurrent measurement. Using organic dyes rhodamine B (Rh B) and nitenpyram (NTP) as model pollutants, the performance of the CoS2-decorated CdS composites for the degradation of model pollutants were evaluated. Among them, the material with the best performance can degrade 99.5% Rh B and 92.5% NTP within 120 min. Furthermore, the catalyst still maintained its high catalytic activity after five cycles. This work provides a new idea for developing efficient and inexpensive hetero-junctions as photo-catalysts.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Jinzhi Jia,Jinhua Zhang,Kailu Guo,Lanyue Zhang,Gening Du,Hao You,Junfeng Huang,Mudong Tu,Hua Li,Yong Peng,Wei Dou,Cailing Xu
Designing highly active and stable electrocatalysts of oxygen evolution reaction (OER) is one of the crucial challenges. In this study, a novel OER electrocatalyst, NiFe-MIL-53 modified with ultra-low rhodium (Rh@NiFe-MIL-53), is successfully prepared via the hydrothermal method. In-situ Raman spectroscopy and electrochemical impedance spectroscopy reveal that the doped Rh accelerates the phase transformation of NiFe-MIL-53 and the in-situ formed Rh@NiFeOOH is the actual active species. More importantly, the enhanced reversibility of electrochemical reconstruction between NiFeOOH and NiFe(OH) 2 after doping Rh is beneficial for improving the electrochemical stability of the catalyst. X-ray photoelectron spectroscopy spectra show the strong electronic interaction between single-atom Rh and Ni/Fe in Rh@NiFeOOH. Furthermore, theoretical calculations confirm that the integration of single-atom Rh into the NiFeOOH successfully reduces the band gap, regulates the d -band center ( ε d ), accelerates the charge transfer, and optimizes the adsorption behavior of oxygen-containing intermediates, thereby lowering the energy barrier of rate-determining steps. Consequently, the optimized Rh@NiFe-MIL-53 exhibits excellent OER activity (240 mV) with a small Tafel slope of 48.2 mV dec −1 and long-term durability (over 1270 h at 10 mA cm −2 and 110 h at 200 mA cm −2 ). This work presents a new perspective on designing highly efficient OER electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2022
·
IF 4.331
Yafeng Wang,Xian Luo,Wenjie Lu,Bin Huang,Yanqing Yang
In this study, β-Ni(OH)2 with a unique flower-like morphology was synthesized through a hydrothermal method. The doping of Rh in β-Ni(OH)2 was achieved by a reduction method. The as-synthesized catalysts were characterized by X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy for the crystal structure, morphology, composition, and chemical state analysis. The electrochemical tests revealed that the doping of Rh can significantly increase the electrocatalytic performance of β-Ni(OH)2 in 1.0 M KOH solution. The methanol oxidation peak current density of Rh-doped β-Ni(OH)2 reached 95 mA cm–2 with a Tafel slope of 40 mV dec–1. The reason for these improvements is that Rh can suppress the phase transformation of NiOOH from β to α. Meanwhile, the electronic structure change of nickel in β-Ni(OH)2 and the defect ratio increase caused by Rh doping are beneficial to methanol oxidation reaction (MOR) catalytic activity. Furthermore, the synergistic effect between Rh and Ni(OH)2 improved the surface activity of β-NiOOH. The doping of Rh in β-Ni(OH)2 is initiative in this work, which provides a new strategy to design highly efficient and cost-effective MOR electrocatalysts for alkaline DMFCs.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Science China-Chemistry
·
2019
·Vol. 62
·期 12
·1710-1719
·
IF 6.085
Wang Guishuo,Luo Ran,Yang Chengsheng,Song Jimin,Xiong Chuanye,Tian Hao,Zhao Zhi-Jian,Mu Rentao,Gong Jinlong
Metal oxide-promoted Rh-based catalysts have been widely used for CO 2 hydrogenation, especially for the ethanol synthesis. However, this reaction usually suffers low CO 2 conversion and alcohols selectivity due to the formation of byproducts methane and CO. This paper describes an efficient vanadium oxide promoted Rh-based catalysts confined in mesopore MCM-41. The Rh-0.3VO x /MCM-41 catalyst shows superior conversion (~12%) and ethanol selectivity (~24%) for CO 2 hydrogenation. The promoting effect can be attributed to the synergism of high Rh dispersion by the confinement effect of MCM-41 and the formation of VO x -Rh interface sites. Experimental and theoretical results indicate the formation of til-CO at VO x -Rh interface sites is easily dissociated into *CH x , and then *CH x can be inserted by CO to form CH 3 CO*, followed by CH 3 CO* hydrogenation to ethanol.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2016
·Vol. 8
·期 13
·2289-2295
·
IF 4.724
Xiaoqin Sun,Shuwei Wang,Cai Shen,Xiaoxiang Xu
Introducing foreign elements is an appealing means to endow wide band gap semiconductors with visible-light responses. Here, we investigated a series of Rh-doped Zn 2 TiO 4 as water reduction photocatalysts. Our results show that Rh doping is effective to improve the visible-light response as well as surface hydrophilicity of Zn 2 TiO 4 . Efficient photocatalytic hydrogen evolution was observed after Rh doping and was found to be compositional dependent. The best performance was recorded for sample Zn 2 Ti 0.96 Rh 0.04 O 4 , with an apparent quantum efficiency of ≈0.74 % under full-range irradiation ( λ ≥250 nm) and ≈0.25 % under visible-light irradiation ( λ ≥420 nm). The light absorption and surface hydrophilicity are likely the controlling factors for the better activity. Theoretical calculations suggest that Rh doping is responsible for a band gap reduction and is due to a newly formed valence band composed mainly of Rh 4d orbitals at the top of the original valence band. The visible-light activity can be attributed to the electron excitations from this new valence band to the conduction band. Graphical Doped semiconductor : Rh doping is an efficient approach to endow wide band gap semiconductor Zn 2 TiO 4 with visible-light responses. Photocatalytic hydrogen production from water was greatly improved after Rh doping both under full-range and visible-light illumination. DFT calculations reveal the critical role of Rh in forming a new valence band. The high photocatalytic activity after doping can be understood as a result of more light absorption as well as improved surface hydrophilicity.
研究领域:
材料科学
·
光催化
·
氢能
·
半导体物理
·
计算材料科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Chen Jiawei,Chen Hongqiu,Cai Xiangbin,Wang Yue,Peng Mi,Sun Bo,Diao Jiangyong,Sun Geng,Ma Ding,Liu Hongyang
Single-atom catalysts have found widespread application in selective hydrogenation reactions partially due to their well-defined active site structures, which ensure exceptional chemical selectivity. However, the limited binding sites on single-atom catalysts hinder their application in hydrogenating larger multidentate substrates (e.g., benzonitrile). In this work, we introduced a heteronuclear Rh-Co dual-atom catalyst stabilized on the defective graphene supports (Rh 1 Co 1 /ND@G), which resolves the activity-selectivity trade-off in nitrile hydrogenation reaction. The Rh 1 site primarily activates H 2 , whereas the Co 1 site synergistically optimizes the adsorption of benzonitrile. The cooperative interaction between Rh-Co dual sites enhances the activation of the C ≡ N bond, significantly reducing the apparent activation energy compared to Rh SACs. The Rh 1 Co 1 /ND@G catalyst achieves exceptional performance under mild reaction conditions, delivering a TOF of 4068 h -1 with >98% dibenzylamine selectivity, surpassing all previous reported heterogeneous catalysts. Remarkably, the Rh 1 Co 1 /ND@G catalyst still maintains robust catalytic performance even after 12 cycles. This work not only presents a breakthrough in dual-atom catalyst design for nitrile hydrogenation, but also opens an avenue for developing high-performance industrial hydrogenation catalysts.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Qi Yang,Pengfei Wang,Chen Li,Benlei Wang,Ying Zheng,Yi Feng,Zidi Miao,Maoshuai Li,Mei-Yan Wang,Shouying Huang,Xinbin Ma
Delineating the geometrical and electronic structure of supported metal is significant for developing heterogeneous hydroformylation catalysts. This study modulated the configuration and charge distribution of Rh to construct highly efficient Rh@SiO 2 catalysts for formaldehyde hydroformylation. The structure sensitivity of Rh species reveals that single-atom Rh can solely catalyze hydrogenation, while Rh aggregates are active for hydroformylation. Moderate Rh nanoclusters (0.98 nm) offered the highest TOF (183 h −1 ) and selectivity (90.8 %) of glycolaldehyde. Electronic effects demonstrate that synergy between Rh 0 and Rh + sites on the cluster is essential to enhancing the reaction. The Rh 0 species function as the adsorption/activation sites for H 2 and formaldehyde, and the Rh + sites act to coordinate PPh 3 and CO to form Rh δ+ (CO) x (PPh 3 ) y active species. This study provides new insights into the design of heterogeneous catalysts and guidance for understanding the structure sensitivity of active metal and hydroformylation mechanism.
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
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhongyao Duan,Kai Deng,Chunjie Li,Mei Zhang,Ziqiang Wang,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Hydrogen evolution reaction (HER) from water electrolysis in alkaline and neutral media provides a possibility to produce pure hydrogen fuel on a large scale. Therefore, the exploration of highly efficient non-Pt HER electrocatalysts is of great significance. Herein, polyaniline (PANI)-coated mesoporous Rh film on Ni foam is controllably fabricated by a micelle-assisted replacement reaction and the subsequent surface modification. Profiting from the synergetic effect of interconnected mesoporous structure, high electrical conductivity of PANI and the modified electronic structure of Rh, the synthesized mRh@PANI film exhibits superior HER electrocatalytic activity and durability in alkaline and neutral electrolytes. To reach a current density of 50 mA cm −2 , low overpotentials of 37 and 69 mV are required in 1 M KOH and 1 M PBS solutions, respectively.
研究领域:
材料科学
·
电化学
✓ 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）