JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Xia Wei,Bing Fang,Tianyao Wang,Hongbin Dai,Song Li
Understanding the metal-support interaction between Rh-B and CeO 2 is essential for enhancing the efficiency of hydrogen generation from hydrous hydrazine. In this study, a series of Rh-B/CeO 2 catalysts were synthesized via a facile wet-chemical reduction method. The Rh-B/(CeO 2 ) 0.7 catalyst exhibits a remarkable 12-fold increase in turnover frequency (TOF) compared to pristine Rh-B catalyst. The strong electronic coupling between Rh-B and CeO 2 was identified as the primary factor driving this significant performance enhancement. This interaction facilitates the formation of oxygen vacancies, promoting hydrazine adsorption and subsequent cleavage of the N-H bond in N 2 H 4 * to form N 2 H 3 *. Our findings emphasize the pivotal role of support engineering in catalyst design for optimizing catalytic performance.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Small
·
2023
·Vol. 20
·期 12
·2307278
·
IF 13.3
Shuo Chen,Yanyan Ma,Liang Zhang,Yuanyuan Zhang,Yuehui Chen,Xiaohua Zhang,Jianhua Yan
Cobalt (Co) is an efficient oxygen reduction reaction (ORR) catalyst but suffers from issues of easy deactivation and instability. Here, it shows that ZrO 2 can stabilize Co through interface electron coupling and enables highly efficient 4e − ORR catalysis. Porous carbon nanofibers loaded with dispersed Co-nanodots (≈10 nm, 9.63 wt%) and ZrO 2 nanoparticles are synthesized as the catalyst. The electron transfer from the metallic Co to ZrO 2 causes interface-oriented electron enrichment that promotes the activation and conversion of O 2 , improving the efficiency of 4e − transfer. Moreover, the simulation results show that ZrO 2 acts like an electron reservoir to store electrons from Co and slowly release them to the interface, solving the easy deactivation problem of Co. The catalyst exhibits a high half-wave potential (E 1/2 ) of 0.84 V, which only decreases by 3.6 mV after 10 000 cycles, showing great stability. Particularly, the enhanced spin polarization of Co in a magnetic field reinforces the interface electron coupling that increases the E 1/2 to 0.864 V and decreases the energy barrier of ORR from 0.81 to 0.63 eV, confirming that the proposed strategy is effective for constructing efficient and stable ORR catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Ting Zhu,Junnan Han,Teng Sun,Jiaming Chen,Sheng Wang,Siyun Ren,Xiaodong Pi,Jun Xu,Kunji Chen
Developing a bifunctional electrocatalyst with remarkable performance viable for overall water splitting is increasingly essential for industrial-scale renewable energy conversion. However, the current electrocatalyst still requires a large cell voltage to drive water splitting due to the unsuitable adsorption/desorption capacity of reaction intermediates, which seriously hinders the practical application of water splitting. Herein, a unique SiOx/Ru nanosheet (NS) material was proposed as a high-performance electrocatalyst for overall water splitting. The SiOx/Ru NSs show superior performance in the hydrogen evolution reaction with a low overpotential of 23 mV (@ 10 mA cm–2) and excellent stability for nearly 200 h (@ 10 mA cm–2) in 1 M KOH. By means of the introduction of SiOx, it is beneficial for balancing the local charge density of the surrounding Ru sites. The suitable electronic coupling between the d-band electrons of Ru and the adsorbed species effectively balances the adsorption and desorption of reaction intermediates on the surface. As a result, the catalyst also exhibits overall water splitting activity with a cell voltage of only 1.496 V to reach the current density of 10 mA cm–2. The present work opens up a new strategy for designing high-performance electrocatalysts for water splitting.
研究领域:
材料科学
·
电化学
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产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 150
·期 9
·2590-2598
·
IF 2.482
Liu Mengyuan,Yan Wenjuan,Wu Jingwei,Wang Shu,Xia Qi,Fang Tianqi,Jin Xin
Selective oxidation of glycerol is one of the most promising routes to produce value-added fine chemicals from biomass. However, achieving good selectivity towards glyceric and lactic acids still remains a grand challenge in this field. A series of unique electronically coupled PtCo catalysts, supported on layered double hydroxides via co-precipitation method, was reported in this work, as they display tunable selectivity toward glyceric acid and lactic acid during glycerol conversion. It is found that the unusual electronic transfer from MgAl hydrotalcite support to cobalt species, leading to high electron binding energy of PtCo sites on catalyst surface. The presence of cobalt components contributes to synergistic enhancement of oxidation activity at electron deficient Pt sites and more critically, weakened Pt–O strength during glycerol conversion. Such unique electronic reconfiguration, as characterized by XRD and XPS spectroscopy, induces two alternative reaction pathways under different reaction temperatures. While Pt–O bonding strength is significantly weakened by strong Co–O affinity at relatively higher reaction temperature (100 °C), such effect is almost negligible at 50 °C. As a result, lactic acid selectivity of 67% was obtained at 100 °C, while glyceric acid selectivity of 65% was achieved at 50 °C, over the bifunctional PtCo/MgAl hydrotalcite catalysts. The design principles reported in this work offer alternative approaches for manufacturing cost-effective catalytic materials for glycerol conversion to various value-added carboxylic acids and derivatives. Graphic Abstract
研究领域:
催化化学
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生物质能
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材料科学
✓ 已验证
DOI
高影响因子
Small
·
2025
·
IF 12.1
Zhibao Wang,Hanqing Gu,Zhanyu Li
Vanadium oxide cathode materials in aqueous aluminum-ion batteries (AAIBs) have an exceptional potential for development because of their high valence and fast electron transfer capability. However, the strong electron–electron Coulomb repulsion in vanadium and its associated electrostatic interactions severely hinder the feasibility of vanadium oxides in AAIBs. The glucose-assisted hydrothermal reduction of monoclinic VO 2 combined with Cu ion doping effectively promotes the self-assembly of VO 2 into nanoflower architectures, enabling precise control over morphology and crystalline structure. When integrated with a 5 m Al(OTF) 3 electrolyte and an Ionic liquid （IL ）-treated Al sheet anode, this full battery demonstrates outstanding electrochemical performance, achieving an initial discharge capacity of 642 mAh·g −1 at 0.4 A·g −1 . Moreover, introducing Cu 3d orbitals effectively enhances the hybridization and electronic coupling effects between the V 3d and O 2p orbitals. Ex situ characterization and diffusion kinetic provide insights into the embedding/de-embedding mechanism of Al 3+ . This work significantly improves the application potential of VO 2 in AAIBs through structural optimization and mechanism studies and provides systematic scientific guidance for the development of vanadium oxide cathode materials.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Wei Li,Yanli Niu,Xiuju Wu,Fawang Wu,Tianhao Li,Weihua Hu
Metal selenides attract great research interest as oxygen evolution reaction (OER) electrocatalysts. Herein, we report heterostructured bimetallic cobalt–iron diselenide nanoparticles with abundant vacancies and strong electronic coupling supported on carbon nanorod (CoSe2/FeSe2@C) as a highly efficient OER electrocatalyst. It is synthesized with a facile templating-engaged synthetic strategy and exhibits outstanding OER catalytic performance including high activity and good durability in alkaline medium. It affords a current density of 10 mA cm–2 at a low overpotential of 291 mV with small Tafel slope of 62 mV dec–1, which significantly outperforms the benchmarking RuO2 catalyst. The outstanding OER performance is found to be arising from its integrated advantages of the modulated electronic structure, abundant active sites, high electric conductivity, and large surface area endowed by its unique heterostructure and composition. This work exemplifies a feasible route to designing heterogeneous nanomaterials and enriches the OER electrocatalytic application of transition metal selenide-based hybrid materials.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
Advanced Energy Materials
·
2025
·
IF 26
Zhiqiang Zheng,Guang Xia,Jiajia Ye,Zhanghua Fu,Tian Qiu,Chuang Chen,Mark J. Biggs,Cheng Hu
Constructing {110}-textured lithium (Li) metal anodes is a promising strategy to extend battery life. While preparation of such anodes has been the subject of a few studies, their focus has been exclusively on thermodynamically-driven (equilibrium) strategies. Through a systematic screening of bath conditions, the study reported here identifies a novel kinetically-driven protocol that enhances the volume fraction of {110} texture by more than fivefold compared to equilibrium approaches. The protocol involves Li deposition at high current densities or low temperatures in a commonly used LiNO 3 -containing ether-based electrolyte. Columnar {110}-oriented grains are formed through a growth rate selection process arising from the stronger electronic coupling and faster electron transfer rate between Li(110) and Li + cations compared to other lattice planes. LiNO 3 plays a crucial role by inhibiting the deposition on the Li(110) plane less than the other planes. Simple bath condition adjustments yield optimized {110}-textured Li anodes with improved plating/stripping homogeneity that suppresses dendrite formation and electrolyte consumption, resulting in extended cycle life in lean-electrolyte full cells. This kinetically-driven approach offers mechanistic insight into Li texture formation and a promising route to high-performance Li metal anodes.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
SUPERCONDUCTOR SCIENCE & TECHNOLOGY
·
2024
·Vol. 37
·期 7
·075003
·
IF 3.7
Qing-Song Yang,Bin-Bin Ruan,Meng-Hu Zhou,Ya-Dong Gu,Kang Zhao,Yun-Qing Shi,Jun-Kun Yi,Le-Wei Chen,Ming-Wei Ma,Gen-Fu Chen,Zhi-An Ren
The hexagonal Mn5Si3-type compounds possess the capability to accommodate specific atoms in the interstices, thereby creating filled Mn5Si3-type structures. In Nb-based Mn5Si3-type system, interstitial atoms like carbon (C) or oxygen (O) have been identified to induce or enhance superconductivity. However, the compounds filled with nitrogen (N) are scarce, and the existence of a N-filled superconductor remains unknown. Here, we report the discovery of a novel ternary nitride superconductor, Nb5Ir3N, synthesized via incorporating N into the electride Nb5Ir3. The crystal structure of Nb5Ir3N conforms to the filled Mn5Si3-type, belonging to the P63/mcm space group (No. 193), with cell parameters a = b = 7.8398(2) Å and c = 5.1108(1) Å. Electrical resistivity and magnetic susceptibility demonstrate that Nb5Ir3N is a type-II superconductor with a Tc of 8.7 K. The estimated lower and upper critical fields are 11.0 mT and 12.16 T, respectively. Moreover, specific heat measurements confirm the bulk superconductivity with enhanced electron–phonon coupling in Nb5Ir3N, as demonstrated by the normalized specific heat jump ΔCe/γTc ∼ 1.59. First-principles calculations emphasize the strong spin–orbit coupling in Nb5Ir3N.
研究领域:
材料科学
·
凝聚态物理
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产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Jian Wang,Junlian Shi,Shuai Wang,Shiguang Fan,Aijun Guo,Zongxian Wang,He Liu
While Pt-based heterogeneous catalysts have been extensively studied for cyclohexane dehydrogenation, the reaction efficiency under low temperatures remains to be resolved. In this paper, ultrafine PtPd alloy nanoparticles homogeneously anchored on nitrogen-doped carbon were synthesized and applied for cyclohexane dehydrogenation. The experimental results indicate that the synergistic effect of Pt-Pd in PtPd/CN catalyst enhances the activity and durability of the catalyst in cyclohexane dehydrogenation compared with Pt/CN and Pd/CN catalysts. The as-prepared catalyst (labeled as Pt 0.75 Pd 0.25 /CN) exhibits an excellent catalytic performance with an initial TOF value of 90.07 mmol·g −1 metal ·min −1 and a 100% H 2 purity for cyclohexane dehydrogenation at 180 °C, exceeding reported values under comparable reaction conditions. Catalyst characterizations and DFT calculations reveal that the electronic coupling effect of Pd and Pt in PtPd/CN catalyst makes the d-band center of Pt active sites closer to the Fermi level, which promotes the specific adsorption/activation of cyclohexane on Pt active sites, thus improving the catalytic performance of cyclohexane dehydrogenation. Under this guidance, the synthesized PtRu/CN and PtIr/CN alloy catalysts exhibited similar enhanced activity in cyclohexane dehydrogenation. This work provides insights into the rational design of efficient and stable Pt-based bimetallic catalysts for cyclohexane dehydrogenation.
研究领域:
化学
·
材料科学
·
催化反应
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 31
·期 9
·2006864
·
IF 16.836
Sisi Liu,Chongjian Zhang,Shuangyuan Li,Yong Xia,Kang Wang,Kao Xiong,Haodong Tang,Linyuan Lian,Xinxing Liu,Ming-Yu Li,Manlin Tan,Liang Gao,Guangda Niu,Huan Liu,Haisheng Song,Daoli Zhang,Jianbo Gao,Xinzheng Lan,Kai Wang,Xiao Wei Sun,Ye Yang,Jiang Tang,Jianbing Zhang
Lead chalcogenide quantum dot (QD) infrared (IR) solar cells are promising devices for breaking through the theoretical efficiency limit of single-junction solar cells by harvesting the low-energy IR photons that cannot be utilized by common devices. However, the device performance of QD IR photovoltaic is limited by the restrictive relation between open-circuit voltages ( V OC ) and short circuit current densities ( J SC ), caused by the contradiction between surface passivation and electronic coupling of QD solids. Here, a strategy is developed to decouple this restriction via epitaxially coating a thin PbS shell over the PbSe QDs (PbSe/PbS QDs) combined with in situ halide passivation. The strong electronic coupling from the PbSe core gives rise to significant carrier delocalization, which guarantees effective carrier transport. Benefited from the protection of PbS shell and in situ halide passivation, excellent trap-state control of QDs is eventually achieved after the ligand exchange. By a fine control of the PbS shell thickness, outstanding IR J SC of 6.38 mA cm −2 and IR V OC of 0.347 V are simultaneously achieved under the 1100 nm-filtered solar illumination, providing a new route to unfreeze the trade-off between V OC and J SC limited by the photoactive layer with a given bandgap.
研究领域:
材料科学
·
光电子学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Hui Liu,Jianing Cheng,Wenjun He,Ying Li,Jing Mao,Xuerong Zheng,Cong Chen,Chunxiang Cui,Qiuyan Hao
Rationally design and exploration of bifunctional electrocatalysts with excellent performance towards water splitting is significant for hydrogen energy economy. Herein, a novel Au/Ni 3 S 2 heterostructure catalyst that was composed of self-supported Ni 3 S 2 nanosheets decorated with Au nanoparticles on Ni foam was fabricated. The bifunctional catalyst exhibited excellent catalytic activities towards oxygen evolution reaction (230 mV @ 10 mA cm −2 ) and hydrogen evolution reaction (97 mV @ 10 mA cm −2 ) in 1 M KOH. The electrolytic tank using the bifunctional catalyst only required 1.52 V to deliver 10 mA cm −2 and sustained for 60 h, outperforming most of advanced bifunctional catalysts. The X-ray absorption fine structure (XAFS) and density functional theory (DFT) calculations validated that the strong electronic coupling at the interface could modulate the electronic structure of Ni 3 S 2 , thereby optimizing the free energies of the adsorbed intermediates. This work provides an atomic-scale insight into the structure-properties relation of a promising heterostructure catalyst for water splitting.
研究领域:
材料科学
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电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 10
·2999-3005
·
IF 4
Jun Li,Ming-Hui Liu,Hong-Yao Shen,Meng-Zhen Liu,Jin-Ting Wu,Bo Zhang
Pursuits of new types of Pb-free heterometallic halides adequate for photovoltaic applications are still urgent but challenging. In this study, by using in situ-produced [(Me)2-(DABCO)]2+ (DABCO = 1,4-diazabicyclo[2.2.2]octane; Me = methyl) cations as structure-directing agents, we successfully constructed a non-perovskite copper iodobismuthate hybrid, namely [(Me)2-(DABCO)]2Cu2Bi2I12 (1), which features discrete [Cu2Bi2I12]4− anionic moieties formed by the building units of [CuI4] tetrahedra and [BiI6] octahedra. UV-Vis diffuse reflectance analyses showed that compound 1 possesses semiconductive behaviors with a narrow optical bandgap of 1.80 eV. More importantly, it exhibits excellent photoelectric switching abilities, and its photocurrent density (2.30 μA cm−2) far exceeds those of some high-performance halide-based counterparts. Different from many heterometallic analogues, noteworthily, it also has dispersive band structure and strong electronic coupling near the Fermi level, resulting in a material with small effective masses that may be responsible for the good photoelectricity. This study may offer new guidance for the design and synthesis of eco-friendly heterometallic halides with unique structures and desirable properties.
研究领域:
材料科学
·
光电化学
·
无机化学
✓ 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）