JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Huimin Mao,Xinyue Qu,Hongsheng Ma,Jingqi Chi,Zhenyu Xiao,Yongming Chai,Zexing Wu,Xiaobin Liu,Lei Wang
Seawater electrolysis is undoubtedly a more sustainable alternative to pure water electrolysis at present. However, it is hindered by the relatively slow kinetics of the oxygen evolution reaction and the detrimental effects of chloride ions in seawater that require resolution. In this study, we developed a straightforward synthesis method and successfully prepared FeNiCoMnCr high-entropy oxide (HEO). The strong coupling among multiple 3d orbitals of the transition metals allows for significant regulation of the catalyst’s electronic structure, enabling oxidation and reduction processes at the active site to spontaneously approach an equilibrium state. Additionally, Lewis acid Cr 6+ selectively adsorbs OH − , further enhancing both activity and stability of the catalyst in alkaline seawater. This research provides valuable insights into utilizing HEOs for seawater electrolysis and elucidates the roles of metals within HEOs.
研究领域:
材料科学
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电化学
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催化科学
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产品关联
DOI
PubMed
高影响因子
Small
·
2023
·Vol. 20
·期 2
·2306464
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IF 13.3
Yijie Wu,Xin Wang,Tiantian She,Taozhu Li,Yunheng Wang,Zhe Xu,Xin Jin,Haiou Song,Shaogui Yang,Shiyin Li,Shicheng Yan,Huan He,Limin Zhang,Zhigang Zou
Transition metals are excellent active sites to activate peroxymonosulfate (PMS) for water treatment, but the favorable electronic structures governing reaction mechanism still remain elusive. Herein, the authors construct typical d-orbital configurations on iron octahedral (Fe Oh ) and tetrahedral (Fe Td ) sites in spinel ZnFe 2 O 4 and FeAl 2 O 4 , respectively. ZnFe 2 O 4 (136.58 min −1 F −1 cm 2 ) presented higher specific activity than FeAl 2 O 4 (97.47 min −1 F −1 cm 2 ) for tetracycline removal by PMS activation. Considering orbital features of charge amount, spin state, and orbital arrangement by magnetic spectroscopic analysis, ZnFe 2 O 4 has a larger bond order to decompose PMS. Using this descriptor, high-spin Fe Oh is assumed to activate PMS mainly to produce nonradical reactive oxygen species (ROS) while high-spin Fe Td prefers to induce radical species. This hypothesis is confirmed by the selective predominant ROS of 1 O 2 on ZnFe 2 O 4 and O 2 •− on FeAl 2 O 4 via quenching experiments. Electrochemical determinations reveal that Fe Oh has superior capability than Fe Td for feasible valence transformation of iron cations and fast interfacial electron transfer. DFT calculations further suggest octahedral d-orbital configuration of ZnFe 2 O 4 is beneficial to enhancing Fe-O covalence for electron exchange. This work attempts to understand the d-orbital configuration-dependent PMS activation to design efficient catalysts.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Nano
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2025
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IF 16
Jing Wu,Guang Yin,Fan-Zhen Jiao,Zhi-Hao Wang,Zhi-Guo Jiang,Zhe Chen,Zhong-Zhen Yu,Jin Qu
Although solar steam generation has been combined with photocatalytic degradation for purifying wastewater, the inherent synergistic effects on enhancing solar-thermal water evaporation and photodegradation are poorly understood. Herein, synergistic solar-thermal and photocatalytic purification of wastewater triggered by photoexcited electron transfer and spin polarization is realized by designing a flow-bed water purification system with a bacterial cellulose/α-Fe2O3 nanodisk/carbon nanotube (BFC) composite film for the continuous solar-thermal evaporation of water and simultaneous photocatalytic degradation of organic pollutants. The photogenerated electrons in the 3dx2–y2 orbitals of the Fe atoms of α-Fe2O3 can transfer to the 2pz orbitals of the C atoms of carbon nanotubes, induced by the work function differences. The separation of photogenerated carriers is enhanced by the built-in electric field and the spin polarization effect, generating more active redox species to improve the photocatalytic degradation performance. Moreover, the photoexcited electrons injected into the carbon nanotubes can participate in solar-thermal conversion via a relaxation process to generate more heat, promoting solar steam generation performance. A flow-bed water purification system is established on the basis of the synergistic solar-thermal/photocatalytic effects for efficiently purifying various wastewater. The purified water is eligible for direct irrigation of crops without any obvious inhibition phenomena.
研究领域:
材料科学
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环境科学
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物理化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Rongchang Ren,Yaning Fu,Mengyao Huang,Zhongjun Li,Youcai Lu,Qingchao Liu
Rare-earth element doping-induced d orbital reconstruction of transition metals emerges as a critical mechanism to overcome the bottleneck of bifunctional catalytic activity in lithium-oxygen (Li O 2 ) batteries. By implementing a cerium doping defect engineering strategy, this study constructs [Ce C Ti] triatomic bridged active centers on MXene surfaces and systematically unravels the cross-scale regulation mechanism governing electronic structure deposition morphology electrochemical performance in MXene-based catalysts. Combined theoretical calculations and experimental characterizations demonstrate that the interfacial charge gradient field enables directional control of Li 2 O 2 epitaxial growth orientation, thereby inducing hierarchical porous structures while synergistically optimizing oxygen species adsorption/desorption kinetics. The [Ce C Ti] bonding disrupts inert electron chains and initiates electronic reconstruction effects, which significantly reduce reaction energy barriers through decoupling of O O bond orbital coupling strength, ultimately achieving self-consistent enhancement of oxygen reduction/evolution reaction activities. This work not only confirms the unique advantage of rare-earth element doping in modulating d orbital electron occupancy of transition metals but also elucidates the interfacial electron-lattice synergy in regulating oxygen electrode reaction pathways.
研究领域:
材料科学
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电化学
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纳米技术
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储能
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表面工程
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催化
✓ 已验证
DOI
高影响因子
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