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| 1 | Asymmetricalπback-donation of hetero-dicationic Mo^(4+)-Mo^(6+)pairs for enhanced electrochemical nitrogen reduction显示文摘The breaking of nonpolar N≡N bond of dinitrogen is the biggest dilemma for electrocatalytic nitrogen reduction reaction(NRR)application,driving electron migration between catalysts and N≡N bond(termed“πback-donation”process)is crucial for attenuating interfacial energy barrier but still remains challenging.Herein,using density functional theory calculations,we revealed that constructing a unique hetero-dicationic Mo^(4+)-Mo^(6+)pair could effectively activate N≡N bond with a lying-down chemisorption configuration by an asymmetrical“πback-donation”process.As a proof-of-concept demonstration,we synthesized MoO_(2)@MoO_(3)heterostructure with double Mo sites(Mo^(4+)-Mo^(6+)),which are embedded in graphite,for electrochemical nitrogen reduction.Impressively,this hetero-dicationic Mo^(4+)-Mo^(6+)pair catalysts display more excellent catalytic performance with a high NH_(3)yield(60.9μg·h^(-1)·mg^(-1))and Faradic efficiency(23.8%)as NRR catalysts under ambient conditions than pristine MoO_(2)and MoO_(3).Operando characterizations using synchrotron-based spectroscopic techniques identified the emergence of a key^(*)N_(2)Hy intermediate on Mo sites during NRR,which indicates that the Mo sites are active sites and the NRR process tends to follow an associative mechanism.This novel type of hetero-dicationic catalyst has tremendous potential as a new class of transition metal-based catalysts with promising applications in electrocatalysis and catalysts for energy conversion and storage. | Hao Tan Qianqian Ji Chao Wang Hengli Duan Yuan Kong Yao Wang Sihua Feng Liyang Lv Fengchun Hu Wenhua Zhang Wangsheng Chu Zhihu Sun Wensheng Yan | 2022 | Nano Research2022，15，4： | 2 |
| 2 | Effect of biochar application method and amount on the soil quality and maize yield in Mollisols of Northeast China显示文摘There have been many studies on soil quality and crop yield using different biochar application amounts,but few studies have focused on the combination of different methods and amounts of biochar application in moderately degraded Mollisols.In this study,the methods of mixing biochar evenly with the soil of the plough layer(0-20 cm depth)[homogeneous biochar application(HO)]and burying biochar above the soil plow pan(under 20 cm depth)(heterogeneous biochar application(HE))were used to reveal how biochar application methods influenced soil quality,crop yield and agronomic characteristics in moderately degraded Mollisols(soil organic matter(SOM),30.33 g kg^(−1)).The biochar application amounts were 0(control),10(level 1),20(level 2),and 40(level 3)t ha^(−1)in both the HO and HE treatments.The results showed that,compared with control,HO3 significantly increased maize yield in the first year,and HO2,HO3,HE2 and HE3 continuously increased maize yield in the next three years but not significantly.HO1 and HE1 had the lowest maize yield.HO2 tended to delay maize leaf senescence.There was a posi-tive linear relationship between soil quality index(SQI)and biochar application amount in HO.Compared with other treatments,the pH,EC,SOM,available phosphorus,sucrase and catalase activities were highest in HO3.However,the effects of HE on soil quality and crop productivity were limited at first but gradually increased with time.Overall,HO3 was beneficial for improving the soil quality and crop productivity in Mollisols for short-term cultivation(3-year),while HE showed an effect over time. | Sihua Yan Shaoliang Zhang Pengke Yan Muhammad Aurangzeib | 2022 | Biochar2022，4，1： | 1 |
| 3 | Enhanced triboelectric output of PDMS-based composite film with bi-material filling and surface patterning显示文摘Triboelectric nanogenerators(TENGs)are highly promising energy-harvesting devices that exhibit considerable potential for use in self-powered wearable electronics.Nano/microfillers and surface microstructure modification have been proposed to improve the triboelectric performance of TENGs.In this work,performance-enhanced flexible polydimethylsiloxane(PDMS)was developed through bi-material(reduced graphene oxide/fluorinated ethylene propylene,rGO/FEP)modification and filtrationmembrane-patterned surface microstructure.The rGO/FEP with high charge-inducing and-trapping capabilities can be used as the dielectric-enhanced filler for improving triboelectricity.Ordered micro-dents of 5–50μm are created on the modified PDMS surface with an increased contact area of TENG.Compared with the pure PDMS,the modified PDMS film-based TENG could deliver a substantial enhancement in power density(0.87 mW cm^(-2))by 28 times.Further,the versatility of this device is demonstrated in human activity monitoring and capacitor charging.This work provided a simple,high-tunability,and scalable approach for improving the output performance of TENGs for biomechanical energy-harvesting devices that can be integrated into self-powering wearable electronics. | LIU Sheng LIAO SiHua LIU Dan ZHAO Rong ZHOU Teng YAN WenYuan WEI KeXiang ZOU HongXiang ZHAO LinChuan | 2023 | Science China(Technological Sciences)2023，66，10： | 0 |
| 4 | Classical spin liquid state in a rhombic lattice metal-organic framework显示文摘Discovering more and new geometrically frustrated systems remains an active point of inquiry in fundamental physics for the existence of unusual states of matter.Here,we report spin-liquid-like behavior in a two-dimensional(2D)rhombic lattice Fe-metal-organic framework(Fe-MOF)with frustrated antiferromagnetism.This Fe-MOF exhibits a high frustration factor f=|θCW|/TN≥315,and its long-range magnetic order is suppressed down to 180 mK.Detailed theoretical calculations demonstrate strong antiferromagnetic coupling between adjacent Fe3+ions,indicating the potential of a classical spin-liquid-like behavior.Notably,a T-linear heat capacity parameter,γ,originating from electronic contributions and with magnetic field independence up to 8 T,can be observed in the specific heat capacity measurements at low-temperature,providing further proof for the spin-liquid-like behavior.This work highlights the potential of MOF materials in geometrically frustrated systems,and will promote the research of exotic quantum physics phenomena. | Sihua Feng Chao Wang Jiyin Zhao Xuguang Liu Chaocheng Liu Zeming Qi Lei Chen Huijuan Wang Minghui Fan Hengli Duan Wensheng Yan | 2024 | Nano Research2024，17，4： | 0 |
| 5 | Highly exposed NiFeO_(x) nanoclusters supported on boron doped carbon nanotubes for electrocatalytic oxygen evolution reaction显示文摘The development of efficient and cost-effective electrocatalysts for oxygen evolution reaction(OER) is crucial for the overall water splitting. Herein, we prepared a highly exposed NiFeO_(x) ultra-small nanoclusters supported on boron-doped carbon nonotubes catalyst, which achieves a 10 mA/cm^(2) anodic current density at a low overpotential of 213 mV and the Tafel slope of 52 mV/dec in 1.0 mol/L KOH, superior to the pristine NiFeO_(x)-CNTs and other state-of-the-art OER catalysts in alkaline media. A combination study(XPS, sXAS and XAFS) verifies that the local atomic structure of Ni and Fe atoms in the nanoclusters are similar to NiO and Fe_(2)O_(3), respectively, and the B atoms which are doped into the crystal lattice of CNTs leads to the optimization of Ni 3d egorbitals. Furthermore, in-situ X-ray absorption spectroscopies reveal that the high valence state of Ni atoms are served as the real active sites. This work highlights that the precise control of highly exposed multicomponent nanocluster catalysts paves a new way for designing highly efficient catalysts at the atomic scale. | Liyang Lv Bing Tang Qianqian Ji Na Li Yao Wang Sihua Feng Hengli Duan Chao Wang Hao Tan Wensheng Yan | 2023 | Chinese Chemical Letters2023，34，3： | 0 |
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