Nano Research
·
2023
·
IF 9.9
Zhang Yufeng,Zhu Wei,Fang Jinjie,Xu Zhiyuan,Xue Yanrong,Pei Jiajing,Sui Rui,Wang Xingdong,Zhang Xuejiang,Zhuang Zhongbin
Electrochemical coupling hydrogen evolution with biomass reforming reaction (named electrochemical hydrogen and chemical cogeneration (EHCC)), which realizes green hydrogen production and chemical upgrading simultaneously, is a promising method to build a carbon-neutral society. Herein, we analyze the EHCC process by considering the market assessment. The ethanol to acetic acid and hydrogen approach is the most feasible for large-scale hydrogen production. We develop AuCu nanocatalysts, which can selectively oxidize ethanol to acetic acid (> 97%) with high long-term activity. The isotopic and in-situ infrared experiments reveal that the promoted water dissociation step by alloying contributes to the enhanced activity of the partial oxidation reaction path. A flow-cell electrolyzer equipped with the AuCu anodic catalyst achieves the steady production of hydrogen and acetic acid simultaneously in both high selectivity (> 90%), demonstrating the potential scalable application for green hydrogen production with low energy consumption and high profitability.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 19
·5686-5693
·
IF 7
Hongjing Wang,Yuqin Liang,Songliang Liu,Xu Mu,Hongjie Yu,Kai Deng,Ziqiang Wang,You Xu,Liang Wang
Coupling the thermodynamically favorable sulfion oxidation reaction (SOR) with the hydrogen evolution reaction (HER) is a promising approach to simultaneously save energy and cost-effectively produce high value-added chemicals and hydrogen. The construction of efficient bifunctional catalysts for SOR–HER electrocatalysis is of significance yet challenging. Here, we propose a dual-nonmetal-doping strategy to construct S and P dual-doped Rh metallene (SP-Rhlene). Benefiting from the combined advantages of dual heteroatom doping and an ultrathin nanosheet structure, SP-Rhlene with a large electrochemical active area and an optimized electronic structure exhibits outstanding HER and SOR activities. A two-electrode system based on optimized SP-Rhlene only needs a cell voltage of 0.385 V at 10 mA cm−2 to generate H2, while transforming S2− into sulfur powder, which further reduces the cost of hydrogen production and protects the ecological environment. This work provides a directive strategy for the rational construction of dual heteroatom doped metallene for energy-saving hydrogen production and environmentally friendly sulfur recovery.
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Nature Chemistry
·
2023
·Vol. 15
·期 11
·1581-1590
·
IF 21.8
Chen Gaoyu,Liu Xiaoyu,An Jiakun,Wang Shibin,Zhao Xiaokun,Gu Zhongzheng,Yuan Caojin,Xu Xiangxing,Bao Jianchun,Hu Han-Shi,Li Jun,Wang Xun
Although their zero- to two-dimensional counterparts are well known, three-dimensional chiral hybrid organic–inorganic perovskite single crystals have remained difficult because they contain no chiral components and their crystal phases belong to centrosymmetric achiral point groups. Here we report a general approach to grow single-crystalline 3D lead halide perovskites with chiroptical activity. Taking MAPbBr 3 (MA, methylammonium) perovskite as a representative example, whereas achiral MAPbBr 3 crystallized from precursors in solution by inverse temperature crystallization method, the addition of micro- or nanoparticles as nucleating agents promoted the formation of chiral crystals under a near equilibrium state. Experimental characterization supported by calculations showed that the chirality of the 3D APbX 3 (where A is an ammonium ion and X is Cl, Br or mixed Cl–Br or Br–I) perovskites arises from chiral patterns of the A-site cations and their interaction with the [PbX 6 ] 4− octahedra in the perovskite structure. The chiral structure obeys the lowest-energy principle and thereby thermodynamically stable. The chiral 3D hybrid organic–inorganic perovskites served in a circularly polarized light photodetector prototype successfully.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2023
·Vol. 34
·期 21
·1-10
·
IF 2.8
Yu Hongquan,Gao Xiao,Huang Chenchen,Liu Shimin,Chen Baojiu,Xu Sai,Zhang Yong,Zhao Hong
CsPbCl 3 and Mn:CsPbCl 3 nanocubes/nanorods were prepared by a hot injection technique. The crystal structure, size and morphology of the CsPbCl 3 and Mn:CsPbCl 3 samples were measured by X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. The edgelengths of the nanocubes and the length and width of the nanorods of CsPbCl 3 are between tens and hundreds of nanometers. The size and morphology of Mn:CsPbCl 3 are similar to those of CsPbCl 3 . The introduction of Mn 2+ ions led to little change in the CsPbCl 3 host structure. Their electrochemical properties for LIB application were tested by cyclic voltammetry, galvanostatic charge–discharge and electrochemical impedance spectroscopy. The introduction of a small amount of Mn 2+ ions can improve the structural stability of CsPbCl 3 during charge–discharge cycles because the Mn 2+ part replaces the Pb 2+ ions of CsPbCl 3 . Thus, Mn:CsPbCl 3 shows high discharge specific capacities, excellent cyclic performance, and lower electrochemical impedance values than CsPbCl 3 in LIB applications.
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Science China-Materials
·
2023
·Vol. 66
·期 9
·3696-3705
·
IF 8.1
Wang Yang,Gao Feng,Zhou Shuai,Hu Po,Fu Jiajun
Lanthanide-doped upconversion nanoparticles (UCNPs) have been extensively investigated owing to their unique advantages. So far, the most favored modality of UCNPs is still the classical Yb–A (where A refers to Er 3+ , Tm 3+ , and Ho 3+ )-coupled nanosystems under 980-nm excitation. However, the frequently used Yb 3+ ion with the single-excited 2 F 5/2 state can barely transfer energy to other acceptors owing to its lack of matched excited levels. Herein, a novel strategy is proposed for energy transfer via Ho 3+ as a bridge ion coupling donor-acceptor pairs (e.g., Yb 3+ –Nd 3+ ), where little direct energy transfer occurs, and the involved energy transport mechanisms are investigated. The findings reveal that long-distance energy transportation can occur in the Ho 3+ sublattice owing to the energy migration capability of Ho 3+ and that Ho 3+ as a bridge ion can realize interparticle energy transfer for upconversion luminescence. Moreover, well-designed NaYbF 4 :40%Ho@NaYF 4 :10%Nd core-shell nanoparticles with multimode responsiveness can emit different colored lights under varying excitation wavelengths, which are demonstrated in high-level anticounterfeiting and information identification. Therefore, this work paves a new way to understand the functionality of the Ho 3+ bridge in energy transfer upconversion and offers strategies for broadening energy transfer pathways and finely manipulating photon upconversion.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2023
·Vol. 39
·期 4
·697-704
·
IF 3.1
Meng Chenchen,Huang Min,Li Yunchao
Covellite copper sulfide nanocrystals(CuS NCs) are typical p-type semiconductors, showing strong optical absorption in the near-infrared(NIR) region thanks to their notable localized surface plasmon resonance(LSPR) properties. However, their LSPR properties and compositions are both highly susceptible to the external environment, which severely limits their practical applications. Until now, it remains a technical challenge to improve the structural and optical stability without sacrificing the LSPR performance of CuS NCs. Herein, to solve such a challenge, CuS@SiO 2 NPs with various silica shell thicknesses(CSNs- X nm) were synthesized in a well-controlled fashion via optimizing reverse microemulsion coating protocol. Compared with the pristine CuS NCs, the as-prepared CuS@SiO 2 NPs exhibited comparable LSPR properties but much higher photostability, enabling resistance to various harsh environments( e.g. , high-power irradiation, strong reduction, and oxidation environment). Impressively, when used in solar-driven interfacial water evaporation, all the CuS@SiO 2 NPs exhibited excellent water evaporation performance with efficiencies beyond 70%(as high as 75.2% for CSN-23 nm) after 20 continuous testing cycles. Evidently, this paper is greatly helpful in better designing and fabricating high-performance plasmonic materials for practical photoelectrical, photothermal, and photocatalytic applications.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 16
·4797-4807
·
IF 7
Lei Qiu,Mengyu Guan,Wei Wang,Maxim S. Molokeev,Sergey P. Polyutov,Zhigao Dai,Guogang Li
Perovskite-based nanocomposites have attracted significant interest due to their potential in interfacial engineering, optical modification, and stability enhancement. However, current understanding of the construction models between perovskites and guest materials is limited, and the design concept of perovskite-based nanocomposites remains unclear. Herein, we thoroughly investigated the effects of amino bridge linkages in attapulgite@perovskite nanocomposites on the crystallization kinetics, optical properties, and stabilities of perovskites. We monitored the difference in structural, compositional, and morphological characteristics. The attapulgite@perovskite nanocomposites with amino bridge linkages exhibited a smaller average size distribution of 23.8 ± 5.8 nm and demonstrated enhanced thermal stability (81% relative PL intensity after one heating–cooling cycle) and photo-stability (84% relative PL intensity after 30 h of ultraviolet light irradiation). These improvements can be attributed to effective passivation by the amino bridge linkages. Our work aims to deepen the understanding of perovskite-based nanocomposite construction and inspire new approaches for modifying their optical properties and enhancing their stability.
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ACS Nano
·
2023
·
IF 17.1
Minxia Zhu,Luwen Zhu,Yuchan You,Mingchen Sun,Feiyang Jin,Yanling Song,Jucong Zhang,Xiaoling Xu,Jiansong Ji,Yongzhong Du
Tumor interstitial pressure represents the greatest barrier against drug diffusion into the depth of the tumor. Biometric nanomotors highlight the possibility of enhanced deep penetration and improve cellular uptake. However, control of their directionality remains difficult to achieve. Herein, we report cysteine-arginine-glutamic acid-lysine-alanine (CREKA)-modified ceria@polydopamine nanobowls as tumor microenvironment-fueled nanoscale motors for positive chemotaxis into the tumor depth or toward tumor cells. Upon laser irradiation, this nanoswimmer rapidly depletes the tumor microenvironment-specific hydrogen peroxide (H2O2) in the nanobowl, contributing to a self-generated gradient and subsequently propulsion (9.5 μm/s at 46 °C). Moreover, the asymmetrical modification of CREKA on nanobowls could automatically reconfigure the motion direction toward tumor depth or tumor cells in response to receptor–ligand interaction, leading to a deep penetration (70 μm in multicellular spheroids) and enhanced antitumor effects over conventional nanomedicine-induced chemo-photothermal therapy (tumor growth inhibition rate: 84.2% versus 56.9%). Thus, controlling the direction of nanomotors holds considerable potential for improved antitumor responses, especially in solid tumors with high tumor interstitial pressure.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Fu-Fei Pu,Yu-Xuan Xiao,Xiong Yang,Fei Yu,Lei Xia,Jiang-Bo Chen,Lu Wu,Jing-Jing Xie,Wen-Ying Zhao,Yu Liu,Li-Ying Wang,Jie Ying,Mei-Jing Liao,Kenneth I. Ozoemena,Ge Tian,Fazhou Wang,Xiao-Yu Yang
Maximization of the utilization of electronic energy and enhancement of mass transfer are important goals in designing high-performance electrocatalytic PtNi nanoalloys. However, realization of such a combination of these properties into Pt based electrocatalysts remains a significant challenge. In an effort targeted at attaining these goals, we prepared several semiconductors (BiVO 4 , CdS and TiO 2 ) modified, gourd-shaped hollow PtNi nanocomposites . We observed that among members of this group, BiVO 4 modified PtNi (denoted as BiVO 4 /PtNi) displays optimal directional electron and mass transfer, which are attributed to the closeness of the work functions of BiVO 4 and PtNi, and a unique gourd-shaped, hollow structure. Moreover, BiVO 4 /PtNi displays remarkable electrocatalytic performance in the hydrogen evolution reaction, in terms of low overpotential of 23 mV to drive the current density of 10 mA cm −2 and a low Tafel slope of 40 mV dec −1 in alkaline natural seawater. Furthermore, this nanocomposite exhibits high stability during a 20-h durability test that greatly exceeds that of commercial Pt/C. The results of this investigation show that new approaches exist for designing novel nanomaterials that have superior performance as electrocatalysts or in other practical applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Huanzheng Yang,Xiaoting Huang,Zhihang Liu,Xu Lin,Qiuyan Chen,Jiawang Li,Chenyue Zhang,Zhi Peng Kan,Zhi Qun Tian,Pei Kang Shen
Ammonia has been emerging as a sustainable and environmentally friendly fuel. However, direct electrochemical ammonia oxidation reaction (AOR) in low-temperature fuel cells seriously suffers from high overpotential and deficient durability. Herein, rhombic dodecahedron nanoframe of platinum iridium copper (PtIrCu) with high-index faceted hyperbranched nanodendrites (RDNF-HNDs) was developed using a one-step self-etching solvothermal method . The framework structure with the high-index facets enables the PtIrCu nanocrystals to expose more effective active sites. They exhibit an ultra-low onset potential of 0.33 V vs. RHE and high mass activity of 26.1 A g PtIr –1 at 0.50 V, which is 140 mV lower and 7.5 times higher than that of commercial Pt/C in the AOR. In situ attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy verifies that AOR on PtIrCu RDNF-HNDs prefers to the NH x dimerization pathways, effectively alleviating the poison of N ads and NO x . The theoretical calculation also shows that both introducing Cu atoms into PtIr alloy and increasing the content of Ir in PtIrCu alloy can reduce the reaction energy barrier of electrochemical dehydrogenation from *NH 2 to *NH. The specific structure of PtIrCu RDNF-NDs provides a new inspiration to solve the critical issue of electrocatalysts for AOR with low activity and durability.
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Small
·
2023
·
IF 13.3
Cong Xie,Xiao Zhang,Hsueh Shih Chen,Ping Yang
The low photoluminescence (PL) efficiency and unstable features of small blue-emitting CsPbX 3 nanocrystals (NCs) greatly limit their applications in optoelectronics field. Herein, the synergistic and post-treatment kinetics are studied to create highly bright and anomalous stable violet (peak position of ≈408 nm) and blue (peak position of ∼ 466 nm) emitting perovskite NCs. Ligand and ion exchange mechanism are systematic studied by the evolution of absorption, PL, and fluorescence lifetime to evaluate ligand bonding, defect engineering, and non-radiative recombination. Didodecyl dimethyl mmonium chloride (DDAC) and CuX 2 post-synergistic treatment created DDAC-CsPbCl 3 -CuCl 2 and DDAC-CsPbCl 3 -CuBr 2 NCs that remained the phase composition, morphology, and size of CsPbCl 3 NCs. The PL efficiencies are drastically increased to 42 and 85% for violet- and blue-emitting NCs, respectively. The stability test indicated that the NCs enable against various harsh conditions (e.g., ultraviolet light irradiation and heat-treatment). The NCs retained their initial PL efficiency after 2 months under ambient conditions and UV light irradiation. These NCs also exhibited high stability after heat-treatment at 120 °C. The emitting NCs embedded in flexible films still revealed bright PL and high stability, suggesting current results provide a new avenue for the application in the field of optoelectronics.
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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Wanting Li,Shiqi Wei,Duankai Wu,Peng Zhang,Guoliang Chen,Binbin Luo,Xiongling Yu,Zhenyu Huang,Feiming Li
2D/3D multidimensional perovskite heterostructures have attracted considerable attention due to their inherent stability and efficient charge transport. However, many challenges remain in fabricating stable 2D/3D multidimensional perovskite heterostructures, such as a precise and convenient pathway to control the perovskite phase with stable interfacial interactions between the 2D and 3D perovskite layers. Therefore, developing a convenient method for the construction of 2D/3D perovskite heterostructures is highly necessary. In this study, we have successfully synthesized stable 2D/3D multidimensional (PEA)2PbBr4 perovskite heterostructures by precisely modulating post cation exchange with cesium oleate (CsOA). As CsOA increased, 2D (PEA)2PbBr4 nanosheets gradually transformed into 3D CsPbBr3, resulting in a multidimensional 2D/3D heterostructure with vivid multi-emission changes. Taking advantage of this precise control process, we explored their potential application in the fluorescent colorimetric detection of Cs+ in soybean oil based on multidimension transformation of 2D (PEA)2PbBr4 nanosheets. This novel strategy not only provides a new approach to constructing 2D/3D perovskite heterostructures but also expands the visual detection strategies for Cs+ sensing.
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