Nano Energy
·
2016
·
IF 11.553
Yingfeng Xu,Ping Lu,Lisong Chen,Chen Zhang,Lingxia Zhang,Xiaohua Zhang,Jianlin Shi
Photoenergy storage catalyst, conventionally constructed by combining a light harvesting component with a charge-storage material, could store partial of photoexcited charge carriers (e − /h + ) under illumination and release them in dark, which is regarded as one of the most promising strategies to compensate the fluctuating availability of solar energy. However, the charge storage efficiency of most reported heterojunctions is quite limited due to the interfacial defects that would quickly quench the photoexcited e − /h + pairs and hinder the charge transfer. Here, through precisely regulating the hydrolysis and condensation kinetics of titanic and molybdate chemical compounds, {Mo(VI)O x } component was incorporated into TiO 2 matrix to construct an artificial atomic-scale heterojunction for photoenergy storage (denoted as Mo-TiO 2 ). In contrast to the conventional nano-scale heterojunction, the absence of defined interfaces in Mo-TiO 2 enables an improved transfer of photoexcited electrons from TiO 2 to {Mo(VI)O x }, leading to an efficient photoenergy storage process under illumination. Then, the stored electrons can spontaneously be released after light turning-off, achieving a dark-continued catalytic activity . The present atomic-scale heterojunction strategy may open up a new dimension for the design and construction of practical photoenergy storage systems.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
Science Bulletin
·
2025
·
IF 21.1
Qing Zeng,Mengyuan Ma,Hui Liu,Lin Xu,Shaonan Tian,Dong Chen,Jing Wang,Jun Yang
Atomic surface engineering for nanostructures significantly contributes to the enhancement of electrocatalysis for a given chemical reaction. However, exploring a facile method to elaborately regulate surfaces at atomic scale remains a grand challenge. Herein, we report the construction of atomically rough surfaces (ARSs) on Au-based binary alloys through a novel and controllable gold (Au)-catalyzed strategy, which involves the first synthesis of Au-based bimetallic nanoalloys, i.e., AuPd and AuAg, and subsequent reduction of another metal ions (Pt, Pd, or Ag) initiated by Au sites on the alloy particle surfaces. By combining ARSs with low-coordinated atoms with ligand effect induced by vicinal Au atoms, the as-prepared ARSs exhibit good activity and durability toward ethanol oxidation reaction (EOR) in an alkaline medium. In particular, the Pd-Pt ARSs on the AuPd alloy particle surface (denoted as AuPd-Pt) exhibit the highest electrocatalytic EOR performance in terms of both specific activity (14.9 mA cm –2 ) and mass activity (28.5 A mg –1 ), surpassing those of their AuPd alloy counterparts, commercial Pd/C catalyst, and most Pd-based electrocatalysts reported recently. In situ Fourier transform infrared (FTIR) spectroscopy reveals that the EOR process on the Pd-Pt ARSs strongly prefers incomplete oxidation, which is further authenticated by the density functional theory (DFT) calculations.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science Advances
·
2025
·Vol. 11
·期 2
·
IF 12.5
Han Gao,Dong He,Zehua Chen,Peili Gao,Dongsheng He,Zhaoning Li,Xusheng Zhang,Jingwei Xiu,Qiang Sun,Shuming Chen,Su-Huai Wei,Shu-Hong Yu,Zhubing He
Owing to the predominant merit of tunable bandgaps, tin-lead mixed perovskites have shown great potentials in realizing near-infrared optoelectronics and are receiving increasing attention. However, despite the merit, there is still a lack of fundamental understanding of the bandgap variation as a function of Sn/Pb ratio, mainly because the films are easy to segregate in terms of both composition and phase. Here, we report a fully stoichiometric synthesis of monocrystalline FAPb1−xSnxI3 nanocrystals as well as their atomic-scale imaging. On the basis of the systematic measurements of the monocrystalline materials, strain and Coulomb interaction–induced atomic ordering was revealed to be responsible for the unusual discontinuous bandgap jumping near x = 0.5 from the expected bowing effect. As a result, both FAPb0.6Sn0.4I3 and FAPb0.4Sn0.6I3 have the lowest bandgaps of around 1.27 electron volts, while that of FAPb0.5Sn0.5I3 is 1.33 electron volts. Correspondingly, their based light-emitting diodes can emit infrared lights with the wavelengths reaching 930 nanometers.
研究领域:
材料科学
·
凝聚态物理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of the American Chemical Society
·
2024
·
IF 14.4
Kai-Yuan Huang,Zhi-Qiang Yang,Ming-Rui Yang,Tian-Shui Chen,Shurong Tang,Wei-Ming Sun,Qiaofeng Yao,Hao-Hua Deng,Wei Chen,Jianping Xie
Metal nanoclusters (MNCs) represent a promising class of materials for catalytic carbon dioxide and proton reduction as well as dihydrogen oxidation. In such reactions, multiple proton-coupled electron transfer (PCET) processes are typically involved, and the current understanding of PCET mechanisms in MNCs has primarily focused on the sequential transfer mode. However, a concerted transfer pathway, i.e., concerted electron–proton transfer (CEPT), despite its potential for a higher catalytic rate and lower reaction barrier, still lacks comprehensive elucidation. Herein, we introduce an experimental paradigm to test the feasibility of the CEPT process in MNCs, by employing Au18(SR)14 (SR denotes thiolate ligand), Au22(SR)18, and Au25(SR)18– as model clusters. Detailed investigations indicate that the photoinduced PCET reactions in the designed system proceed via an CEPT pathway. Furthermore, the rate constants of gold nanoclusters (AuNCs) have been found to be correlated with both the size of the cluster and the flexibility of the Au–S framework. This newly identified PCET behavior in AuNCs is prominently different from that observed in semiconductor quantum dots and plasmonic metal nanoparticles. Our findings are of crucial importance for unveiling the catalytic mechanisms of quantum-confined metal nanomaterials and for the future rational design of more efficient catalysts.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2024
·Vol. 20
·期 50
·2405567
·
IF 13
Minghui Cui,Rongjing Guo,Feilong Wang,Yansong Zhou,Wenqi Zhao,Yanjing Liu,Qiongrong Ou,Shuyu Zhang
Industrial water electrolysis typically operates at high current densities, the efficiency and stability of catalysts are greatly influenced by mass transport processes and adhesion with substrates. The core scientific issues revolve around reducing transport overpotential losses and enhancing catalyst-substrate binding to ensure long-term performance. Herein, vertical Ni-Co-P is synthesized and employed plasma treatment for dual modification of its surface and interface with the substrate. The (N)Ni-Co-P/Ni 3 N cathode exhibits an ultra-low overpotential of 421 mV at 4000 mA cm −2 , and the non-noble metal system only requires a voltage of 1.85 V to reach 1000 mA cm −2 . When integrated into an anion exchange membrane (AEM) electrolyzer, it can operate stably for >300 h at 500 mA cm −2 . Under natural light, the solar-driven AEM electrolyzer operates at a current density up to 1585 mA cm −2 with a solar-to-hydrogen efficiency (SHT) of 9.08%. Density functional theory (DFT) calculations reveal that plasma modification leads to an “atomic-scale soldering” effect, where the Ni 3 N strong coupling with the Co increases free charge density, simultaneously enhancing stability and conductivity. This research offers a promising avenue for optimizing ampere-level current density water splitting, paving the way for efficient and sustainable industrial hydrogen production.
研究领域:
材料科学
·
能源化学
·
电催化
·
氢能源
✓ 已验证
DOI
高影响因子
Chem
·
2023
·
IF 23.5
Na Yao,Hongnan Jia,Juan Zhu,Zhaoping Shi,Hengjiang Cong,Junjie Ge,Wei Luo
The development of highly efficient and stable electrocatalysts toward the acidic oxygen evolution reaction (OER) is essential for the practical application of proton-exchange membrane water electrolyzers. Although Ru oxides possess remarkable initial activity toward the acidic OER due to the kinetically favorable lattice oxygen oxidation mechanism pathway, the soluble high-valence oxygen-vacancy intermediate (∗Vo-RuO 4 2− ) may accelerate the dissolution of Ru species, leading to dramatically decreased activity and unsatisfied long-term stability. Here, we developed a robust metal-organic framework anchored strategy by stabilizing atomically isolated Ru oxide on UiO-67-bpydc with strong coordinating pyridine ligands. Theory calculations and experimental results including in situ Raman, X-ray absorption spectroscopy, and 18 O-labeled differential electrochemical mass spectrometry reveal that the Ru–N bonds between Ru oxide and UiO-67-bpydc could not only accelerate the participation of lattice oxygen during the OER process but also stabilize the soluble ∗Vo-RuO 4 2− intermediate, which contribute to the enhanced OER performance and long-term stability of up to 115 h.
研究领域:
电催化
·
材料化学
·
能源科学
·
无机化学
·
物理化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Ziyu Kuai,Yibing Huang,Fengjie Hao,Wantong Jiang,Mengmeng Niu,Yu qin,Ao Song,Yuran Deng,Youzhong Wan,Quan Luo
Atomic precision synthesis and modulation of nanozymes are critical for evaluating their performance and developing functional applications. Herein, we developed an in situ strategy for the controlled synthesis of gold clusterzymes (AuCEs) within the confined cavities of the protein scaffolds. Using a stable dodecameric protein (SP1) as a ligand, we fused a short peptide containing the CCY sequence (SP1-CCY) to the N-terminus of SP1, which is located within its cyclic structure. In this design, cysteine and tyrosine synergistically chelate and reduce Au ions, while the confined protein structure restricts cluster growth, leading to the formation of a 25-gold atom (Au25) nanocluster with strong fluorescence and peroxidase-like activity. Unlike chemical ligands, protein scaffolds offer atomic-level precision and allow for site-specific modulation of the local environment through rational mutations, such as L9D, L9I, and E73I/L9I. This allows precise control of both fluorescence and enzymatic activity via protein engineering. Additionally, heteroatom doping of the Au core with copper endows the AuCEs with significant superoxide dismutase-like activity. Antioxidant assays demonstrate that the optimized AuCEs exhibit potent reactive oxygen species scavenging activity, providing significant protection to Caenorhabditis elegans from oxidative stress and highlighting their potential as therapeutic candidates for aging-related diseases.
研究领域:
纳米医学
·
生物材料学
·
分子生物学
·
老年病学
·
抗氧化治疗
·
纳米酶
·
转化医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
·
2025
·
IF 5.5
Tinglei Wang,Lu Zhang,Laipeng Sun,Jiaqi Zhao,Yuan Wang,Zexing Qu,Yu Wang
The site-specific boron-doped graphitic carbon nitride (B-g-C3N4-20) has been synthesized via precise solid-state synthesis methods. Thermodynamic analysis indicates that its excellent reproducibility stems from similar activation energies of the dehydration and condensation reactions involving phenylboronic acid and melamine, as well as the dehydration polymerization of melamine with cyanuric acid. It allows both reactions to occur concurrently, leading to the orderly arrangement of intercalated molecules within the carbon nitride nanosheets, facilitating targeted boron incorporation. The boron atoms of the intercalated molecules not only form triple bonds with nitrogen atoms, horizontally arranging in an ordered manner, but also vertically interact with tertiary nitrogen atoms of the carbon nitride nanosheets. This dual-directional ordered interaction between boron and nitrogen creates atomic-scale p–n junctions at the microscopic level and exhibits a pronounced p–n junction effect at the macroscopic level. Such structural characteristics significantly improve the transport pathways for photogenerated charge carriers, resulting in a remarkable increase in photocatalytic performance with a hydrogen peroxide production rate 30 times higher than that of pure graphitic carbon nitride under neutral conditions. This work not only offers additional perspectives for advancing solid-state synthesis methods but also serves as an innovative example for the development of other functional materials.
研究领域:
材料科学
·
纳米技术
·
催化
·
固态化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Science China-Materials
·
2017
·Vol. 60
·期 11
·1121-1128
·
IF 3.956
Yang Hongchao,Wang Changhong,Hu Feng,Zhang Yejun,Lu Huan,Wang Qiangbin
The synthesis of atomic-scale metal catalysts is a promising but very challenging project. In this work, we successfully fabricated a hybrid catalyst of Ptc/Ni(OH) 2 with atomic-scale Pt clusters uniformly decorated on porous Ni(OH) 2 nanowires (NWs) via a facile room-temperature synthesis strategy. The as-obtained Pt c /Ni(OH) 2 catalyst exhibits highly efficient hydrogen evolution reaction (HER) performance under basic conditions. In 0.1 mol L −1 KOH, the Pt c /Ni(OH) 2 has an onset overpotential of ~0 mV vs. RHE, and a significantly low overpotential of 32 mV at a current density of 10 mA cm −2 , lower than that of the commercial 20% Pt/C (58 mV). The mass current density data illustrated that the Pt c /Ni(OH) 2 reached a high current density of 6.34 Amg
−1 Pt
at an overpotential of 50 mV, which was approximately 28 times higher than that of the commercial Pt/C (0.223 A mg
−1 Pt
) at the same overpotential, proving the high-efficiency electrocatalytic activity of the as-obtained Pt c /Ni(OH) 2 for HER under alkaline conditions.
研究领域:
材料科学
·
电化学
·
纳米催化
·
能源材料
·
物理化学
✓ 已验证
DOI
高影响因子
Small
·
2025
·
IF 12.1
Qiqiong Ren,Pei Wang,Nan Zhang,Guojun Zhou,Xian-Ming Zhang
Organic–inorganic hybrid materials face significant barriers to large-scale commercialization, primarily stemming from their intrinsic vulnerability to moisture-triggered hydrolytic degradation. Herein, an ultra-stable 2D copper(I) iodide, Cu 6 I 6 (26dmpz) 3 , is engineered through a synergistic waterproofing strategy that integrates atomic-level passivation and surface-interface hydrophobicity. N-metal coordination in Cu 6 I 6 (26dmpz) 3 (26dmpz = 2,6-dimethylpyrazine) passivates H-bond donors at atomic-level, blocking hydrolytic degradation induced by N─H···O interactions. Its methyl-dominated non-polar surface and “hydrogen-bond-free” contribute to low surface energy (37.68 mJ m −2 ) and polarity (4.09 mJ m −2 ), minimizing water adsorption, as corroborated by a 130.8° contact angle. The 2D corrugated groove structure creates a physical barrier against water penetration at solid–liquid interfaces. This endows Cu 6 I 6 (26dmpz) 3 with exceptional water stability, preserving its structure and luminescence after 30 days in water. Moreover, it shows bright orange–red emission (616 nm) with strong blue-light response, attributed to halide/metal-to-ligand charge transfer. The fabricated white LED exhibits an ultra-high color rendering index (CRI = 89.9), showing tremendous potential for high-quality solid-state lighting.
研究领域:
无机化学
·
材料科学
·
光功能材料
·
固体化学
·
纳米材料
·
光电转换
·
环境稳定性
·
照明技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2025
·
IF 14.1
Siqi Qiu,Hao Wan,Yuechao Yao,Xiao Xu,Zhangjian Li,Yongbiao Mu,Biaolin Peng,Hongliang Wu,Jizhao Zou,Lin Zeng
Iron-nitrogen-carbon (Fe-N-C) materials are promising non-precious metal catalysts for the oxygen reduction reaction (ORR), yet their long-term stability remains a critical challenge due to the dissolution of Fe-based active sites and corrosion of the carbon support. Here, a Fe-Zr dual-atom carbon-based catalyst (Fe,Zr-NC) via a one-step solid-state synthesis method is reported. The introduction of atomically dispersed Zr–N units adjacent to Fe–N 4 centers creates a dual-metal coordination structure that modulates the local electronic environment of Fe and weakens * OH adsorption, which is the rate-limiting step in the ORR process. Density functional theory (DFT) calculations reveal that the Fe–Zr synergy positions the catalyst near the apex of the ORR activity volcano. Extended experimental EXAFS confirms a Fe–Zr distance of ≈3.30 Å, closely matching the theoretical optimum (≈3.39 Å). As a result, Fe, Zr-NC achieves a high half-wave potential (0.891 V vs reversible hydrogen electrode (RHE)) with negligible activity loss over 5000 cyclic voltammetry cycles, outperforming commercial Pt/C. In zinc–air batteries, the catalyst delivers a peak power density of 185.7 mW cm −2 and operates stably for over 453 h. This work highlights the importance of dual-atom synergy in tuning intermediate binding energies and provides design principles for next-generation ORR electrocatalysts.
研究领域:
电催化
·
材料化学
·
能源化学
·
纳米材料
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Shuai Cui,Enze Xu,Lei Wang,Xin Song,Kelong Liu,Na Liu,Xiaolong Yan,Mingyao Li,Yusen Yang,Min Wei
Hydroformylation, a pivotal industrial reaction heavily reliant on Rh-based catalysts, remains limited by Rh scarcity and cost. While Co-based catalysts are potential alternatives, they still face dual challenges of insufficient activity and stability. In this work, Co-based intermetallic catalysts (CoMoIMC and CoWIMC) were synthesized through a layered double hydroxide precursor strategy. During propylene hydroformylation, CoMoIMC exhibited a butyraldehyde production rate of 105 mmol·g −1 ·h −1 (97 % selectivity) with >90 % activity retention over 10 cycles under mild conditions (140 °C, 4.5 MPa), outperforming conventional CoAl 2 O 3 by 2.4-fold. Reactant-TPD experiments and DFT calculations revealed that the ordered Co 3 Mo/Co 3 W structures altered CO adsorption from hollow to top sites, reducing the desorption energy from 29.7 to 19.7 kJ·mol −1 and lowering the CO insertion barrier from 1.28 to 1.09 eV. This work proposes a new strategy for preparing highly active and stable non-noble metal hydroformylation catalysts, which has a promising potential for industrial applications.
研究领域:
催化化学
·
材料化学
·
工业化学
·
表面科学
·
反应机理研究
✓ 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）