Journal of Materials Chemistry A
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2025
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IF 9.5
Chenyang Duan,Hao Zhang,Zhiwei Hu,Zhenya Li,Wenjie Bian,Chao Jing,Jian-Qiang Wang,Linjuan Zhang
Modulating the configurational entropy of materials is an effective strategy to develop efficient and robust electrocatalysts for the oxygen evolution reaction (OER) in clean energy technologies. However, the impact of configurational entropy on catalytic activity has received limited attention. In this study, we systematically investigate a class of alloy catalysts composed of Cr, Mn, Fe, Co, and Ni, as a function of Ni content to modulate the configurational entropy to 1.50R (high-entropy alloy, Ni-HEA), 1.23R (medium-entropy alloy, Ni-MEA), and 0.66R (low-entropy alloy, Ni-LEA), where R is 8.314 J (mol−1 K−1). In situ Raman spectroscopy reveals that increased configurational entropy facilitates the formation of the OER active γ-NiOOH phase on the alloy surface. This transition leads to a significant decrease in the OER overpotentials and Tafel slopes. The optimized Ni-HEA exhibits an overpotential of only 217 mV at 10 mA cm−2, and demonstrates prolonged operational stability for 600 hours under industrial conditions. This work enhances our understanding of the impact of configurational entropy on catalytic activity and offers a novel approach for the rational design of porous high-entropy catalysts with improved OER efficiency.
研究领域:
材料科学
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电化学
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清洁能源技术
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产品关联
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2017
·Vol. 19
·期 36
·24689-24695
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IF 4.123
Minghai Yao,Peng Wu,Shuang Cheng,Lufeng Yang,Yuanyuan Zhu,Mengkun Wang,Haowei Luo,Bangfen Wang,Daiqi Ye,Meilin Liu
α-V2O5 nanowires with a layered structure have been fabricated through a two-step procedure. When measured as a pseudo-capacitive electrode with a three-electrode configuration in 1 M Na2SO4 aqueous solutions, α-V2O5 exhibits ideal capacitive characteristics with a specific capacitance of ∼238 F g−1 at a high current of 2 A g−1, but poor cycling stability with a continuous drop in the first 2000 cycles before it is maintained. To find possible solutions towards this problem, the energy storage behavior of the α-V2O5 electrode has been carefully investigated. In situ Raman analysis suggests that it is electrolytic hydrated cations [Na(H2O)n]+ rather than anions (SO42−) that are involved in the energy storage process through reversible adsorption/desorption on the surface or intercalation/deintercalation at the interlayer of the (001) planes accompanied by interlayer spacing expansion/contraction. Moreover, the electrochemical quartz crystal microbalance results indicate that, besides a reversible mass change, there is a continuous mass loss that may originate from slow dissolution of V2O5, which should bear the main responsibility for the poor stability (initial dramatic drop). Hence, how to inhibit dissolution, such as by coating or adding additives in the electrolyte, is found to be the key approach to improve the stability of V2O5 based electrodes.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL EDUCATION
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2025
·
IF 2.9
Handong Jiao,Qiang Liu,Shuqiang Jiao
High-temperature molten-salt electrochemistry (MSE) is a branch of chemistry that has applications across various sectors, including the chemical, metallurgical, materials, nuclear, and even deep space exploration industries. Consequently, it is significant for chemistry undergraduates to engage in experimental training focused on high-temperature MSE. In this study, we developed an instrument for in situ Raman spectroscopic analysis of electrode processes in molten salts. Utilizing this instrument, we designed a rigorous and feasible experimental scheme, along with a comprehensive evaluation method. The integration of in situ Raman spectroscopy and our experimental protocol enables students to gain profound insights into molten-salt electrode processes while deepening their understanding of the underlying reaction mechanisms. Notably, this pedagogical approach not only cultivates students’ interest in chemistry but also enhances their scientific reasoning skills and exposes them to cutting-edge knowledge.
研究领域:
化学教育
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物理化学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lixiong Xu,Yifan Yang,Chenyue Li,Rongqian Ning,Jun Ma,Mengqin Yao,Shuo Geng,Fei Liu
The electrocatalytic glycerol oxidation reaction (GOR) is an efficient way to reduce the overpotential of the anodic reaction of electrocatalytic water splitting with abundant high-value byproducts. However, it has always been difficult to reveal a clear reaction path and real active site during the electrocatalytic glycerol oxidation reaction (GOR) process. In this work, NiOOH/Ni 3 S 2 /NF, a model catalyst was synthesized by the two-step method, and the reaction path of the electrocatalytic oxidation of glycerol on NiOOH/Ni 3 S 2 /NF was clearly unveiled by the in situ infrared and Raman analysis. In addition, the TEM after GOR and in-situ Raman intuitively demonstrated that the NiOOH was the real active site during the GOR process. Consequently, the synthesized NiOOH/Ni 3 S 2 /NF catalyst achieved a current density of 10 mA cm −2 at 1.227 V vs . RHE and obtained a high formic acid Faraday efficiency of 97.7 % at a low potential of 1.4 V vs . RHE. This work demonstrates an effective method for unveiling the GOR mechanism and the other relevant electrocatalytic reaction processes.
研究领域:
电化学
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催化科学
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产品关联
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Hongyu Liang,Xiaojie Xia,Manqiang Liu,Shijing Zou,Tianqiang Yin,Hongfei Li,Yanhu Zhang,Chunying Min,Yongfeng Bu
High load-bearing capacity is one of the crucial indicators for liquid superlubricants to move toward practicality. However, some of the current emerging systems not only have low contact pressures but also are highly susceptible to further degradation due to water adsorption and even superlubricity failure. Herein, a novel choline chloride-based ionic liquid analogues (ILAs) of a superlubricant with triethanolamine (TEOA) as the H-bond donor is reported for the first time; it obtains an ultralow coefficient of friction (0.005) and high load-bearing capacity (360 MPa, more than 2 times that of similar systems) due to adsorption of a small amount of water (<5 wt %) from the air. In situ Raman combined with 1H NMR and FTIR techniques reveals that adsorbed water competes with the hydroxyl group of TEOA for coordination with Cl–, leading to the conversion of some strong H-bonds to weak H-bonds in ILAs; the localized strong H-bonds and weak H-bonds endow the ILAs with high load-bearing capacity and the formation of ultralow shear-resistance sliding interfaces, respectively, under the shear motion. This study proposes a strategy to modulate the interactions between liquid species using adsorbed water from air as a competing ligand, which provides new insights into the design of ILA-based macroscopic liquid superlubricants with a high load-bearing capacity.
研究领域:
材料科学
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摩擦学
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化学工程
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产品关联
DOI
PubMed
高影响因子
MethodsX
·
2019
·
IF 0
Chengyuan Liu,Zhiwei Liu,Hongkun Niu,Cong Wang,Zhaowen Wang,Bingliang Gao,Jingjing Liu,Mark Taylor
We provide a method for preparation of binder-free cathode for rechargeable aluminum-ion batteries (AIBs). Ultrasonicated natural graphite (u-NG) flakes in N-methylpyrrolidone (NMP) is drop-casted to a carbon fiber cloth (CFC) to obtain binder-free u-GF@CFC cathode for AIBs. We also provide an in-situ Raman spectral technology and the corresponding in-situ Raman cell to determine the mechanism of intercalation/deintercalation reactions of the chloroaluminate ions at cathode of AIBs. The in-situ Raman spectra are recorded using a Raman spectrometer combined with a potentiostat/galvanostat model electrochemical workstation. • A simple preparation method of a binder-free u-GF@CFC cathode is suggested. • The u-GF@CFC cathode is obtained by drop-casting ultrasonicated graphite flakes on the surface and internal gaps of the carbon fiber cloth. • The method includes the in-situ Raman spectral technology and the corresponding in-situ Raman cell.
研究领域:
电化学
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能源材料
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纳米材料
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电池技术
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原位表征
✓ 已验证
DOI
JOURNAL OF RARE EARTHS
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2025
·
IF 7.2
Bolin Zhao,Rana Muhammad Irfan,Chuhao Liu,Shamraiz Hussain Talib,Azhar Mahmood,Li Niu
Rare-earth based transition metal oxides have proved to be the most promising candidates in the exploration of non-precious oxygen evolution reaction (OER) catalysts. However, the knowledge regarding their active sites and electrocatalytic mechanism is very limited due to their different crystallization behaviors and there are still big challenges in the efficient coupling of transition and rare-earth metals with full utilization of active sites. To improve and stabilize OER catalysis, we developed the core-shell CeO 2 @CoNiO 2 nanoplates (NPLs) for enhanced and stable OER catalysis. Surprisingly, CeO 2 shell regulates the electronic structure of CoNiO 2 core and increases the number of active sites and oxygen vacancies to achieve high electrochemical performance in a three-electrode system. Compared with CoNiO 2 nanoparticles, the developed core-shell NPLs exhibit favorable performance with an overpotential of only 206 mV at 10 mA/cm 2 and robust electrochemical stability of 500 h at 10 mA/cm 2 and 300 h at 50 mA/cm 2 . In situ Raman spectroscopy unveils that CeO 2 @CoNiO 2 is structurally more stable than CoNiO 2 , which is consistent with its performance persistence. Besides, theoretical calculations confirm that the Ce shell serves as the active centers for OER, and the formed core-shell metal oxides NPLs promote the adsorption and dissociation of water, thus causing the fast generation of O 2 . This work provides a new perspective for designing highly active core-shell structure of mixed metal oxides of transition and rare-earth metals for OER.
研究领域:
电化学
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材料科学
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催化
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纳米技术
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能量转换
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Pengyan Wang,Chengmei Ding,Zubing Huang,Jiwei Lv,Meiyan Li,Shiwei Zhang,Xupo Liu,Shichun Mu
For a single-substance catalyst, due to the different adsorption/desorption kinetics of metallic (cationic) and nonmetallic (anionic) sites, it typically catalyzes hydrogen evolution in a single-active-site manner, which greatly limits the activity of catalysts. Thus, herein, we simultaneously activate the anion (P) and cation (Ni) sites in nickel phosphide (Ni2P) and generate highly active P(Ni) dual sites through the substrate effect of NiS2–NiS heterogeneous structures. Theoretical calculation results combined with in situ Raman spectroscopy unveil that the NiS2–NiS substrate effectively regulates the charge distribution to concentrate around the P atom, therefore resulting in Ni and P synergistic dual active sites for water adsorption, water dissociation, and H* adsorption. Accordingly, the dual active site formed enables the Ni2P/NiS2–NiS electrocatalyst to only require an overpotential of 75 mV to achieve a current density of 10 mA cm–2 in alkaline media, very close to the Pt-group noble metal catalyst. This work highlights the critical regulatory role of substrates in activating the anion–cation dual active site in the single metal/intermetallic compound (such as metal phosphides, sulfides, nitrides, carbides, borides, and silicides) that promotes catalytic performance.
研究领域:
材料化学
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电催化
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能源科学
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纳米材料
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物理化学
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表面科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Ying Li,Yanyan Wu,Hongru Hao,Mengke Yuan,Zhe Lv,Lingling Xu,Bo Wei
Oxygen evolution reaction (OER) is a key step for electrochemical water splitting and understanding the surface reconstruction of OER pre-catalysts is of vital importance. Herein, hybrid Ni 5 P 4 @FeP nanosheet arrays were evaluated as promising OER pre-catalysts. The dynamic surface evolution was probed by in situ Raman spectroscopy, which revealed that Ni 5 P 4 @FeP was rapidly reconstructed to NiFe 2 O 4 during the anodic scan. The structural instability of amorphous NiFe 2 O 4 led to partial reconstitution to Ni/FeOOH at high oxidation potentials. As-formed Ni/FeOOH@NiFe 2 O 4 hybrid with high structural reversibility was established as a truly active species, which exhibited excellent alkaline OER performance with a low overpotential of 205 and 242 mV under current densities of 10 and 100 mA cm −2 , respectively. This work provides a facile strategy to in situ construct an amorphous spinel/oxyhydroxide hybrid structure using electrochemical activation that holds strong promise for potential application in electrochemical water splitting and related energy devices.
研究领域:
电化学
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材料科学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Hao Liu,Jianjun Chen,Ya Wang,Shangchao Xiong,Ziang Su,Yun Wang,Wenhao Yang,Xuefeng Chu,Weinan Yang,Yue Peng,Wenzhe Si,Junhua Li
A series of Sm-doped Co 3 O 4 catalysts for the N 2 O direct catalytic decomposition were synthesized by the sol–gel method using citric acid as a chelating agent and urea as a combustion agent. The doping of Sm significantly altered the activity of N 2 O decomposition on the Co 3 O 4 catalyst. Sm was incorporated into the Co 3 O 4 matrix, leading to the distortion of Co 3 O 4 lattice with the spinel configuration maintained. Sm-doping can effectively promote the oxygen vacancy generation, and the electron interaction between Co and Sm species occurred as the Co 3+ + Sm 2+ ↔ Co 2+ + Sm 3+ redox cycle. Combined with in situ Raman and in situ NAP-XPS results proposed that this redox cycle is the main reason that the Sm-doping accelerates the high-efficiency N 2 O decomposition.
研究领域:
催化
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材料科学
·
环境化学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Wenxuan Zhang,Chuqian Xiao,Yuhang Li,Chunzhong Li
5-Hydroxymethylfurfural (HMF) electrooxidation for 2,5-furandicarboxylic acid (FDCA) production has become a sustainable method for value-added products at the anode. Here, an amorphous NiMo composite oxide supported on nickel foam (NF) is fabricated for HMF electrooxidation (HMFOR) via one-step electrodeposition. The synthesized NiMo/NF delivers 98.3% FE toward FDCA at 1.5 VRHE and maintains FE above 90% during 10 h. In situ Raman spectroscopy proves the formation of the active species Ni3+-OOH during the reaction process. Due to the introduction of high-valent Mo6+, the Ni3+ active species can be stabilized and the adsorption of aldehyde in HMF can be promoted during the reaction process, thus enhancing the FDCA electrosynthesis performance.
研究领域:
材料科学
·
电化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 39
·2302530
·
IF 13.3
Xiaotong Li,Minkai Qin,Xiuju Wu,Xiangzhou Lv,Jianghao Wang,Yong Wang,Hao Bin Wu
Electrochemical CO 2 reduction reaction (CO 2 RR) is a promising strategy for waste CO 2 utilization and intermittent electricity storage. Herein, it is reported that bimetallic Cu/Pd catalysts with enhanced *CO affinity show a promoted CO 2 RR performance for multi-carbon (C2+) production under industry-relevant high current density. Especially, bimetallic Cu/Pd-1% catalyst shows an outstanding CO 2 -to-C2+ conversion with 66.2% in Faradaic efficiency (FE) and 463.2 mA cm −2 in partial current density. An increment in the FE ratios of C2+ products to CO for Cu/Pd-1% catalyst further illuminates a preferable C2+ production. In situ Raman spectra reveal that the atop-bounded CO is dominated by low-frequency band CO on Cu/Pd-1% that leads to C2+ products on bimetallic catalysts, in contrast to the majority of high-frequency band CO on Cu that favors the formation of CO. Density function theory calculation confirms that bimetallic Cu/Pd catalyst enhances the *CO adsorption and reduces the Gibbs free energy of the C C coupling process, thereby favoring the formation of C2+ products.
研究领域:
电化学
·
材料科学
·
催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）