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| 1 | Engineering the Coordination Sphere of Isolated Active Sites to Explore the Intrinsic Activity in Single-Atom Catalysts显示文摘Reducing the dimensions of metallic nanoparticles to isolated,single atom has attracted considerable attention in heterogeneous catalysis,because it significantly improves atomic utilization and often leads to distinct catalytic performance.Through extensive research,it has been recognized that the local coordination environment of single atoms has an important influence on their electronic structures and catalytic behaviors.In this review,we summarize a series of representative systems of single-atom catalysts,discussing their preparation,characterization,and structure-property relationship,with an emphasis on the correlation between the coordination spheres of isolated reactive centers and their intrinsic catalytic activities.We also share our perspectives on the current challenges and future research promises in the development of single-atom catalysis.With this article,we aim to highlight the possibility of finely tuning the catalytic performances by engineering the coordination spheres of single-atom sites and provide new insights into the further development for this emerging research field. | Xin Wu Huabin Zhang Shouwei Zuo Juncai Dong Yang Li Jian Zhang Yu Han | 2021 | Nano-Micro Letters2021，13，9： | 4 |
| 2 | Different mechanisms of improving CH_(3)NH_(3)PbI_(3) perovskite solar cells brought by fluorinated or nitrogen doped graphdiyne显示文摘Fluorinated and nitrogen-doped graphdiyne(F/N-GDY)have been used in the active layer of perovskite solar cells(PSCs)for the first time.The introduction of heteroatoms turns out to be an effective method for boosted solar cells performance,which increases by 32.8%and 33.0%,better than the pristine or GDY doped PSCs.The enhanced performance can be attributed firstly to the superiority of F/N-GDY originated from the unique structure and optoelectronic properties of GDY.Then,both can further reduce surface defects and improve surface and bulk crystallinity than pristine GDY.What's more,efficiency increase caused by F-GDY is mainly attributed to the improvement of fill factor(FF),while the higher short-circuit current(Jsc)plays more important role by N-GDY doping.Most importantly,the detailed mechanism brought about by doping of F-GDY or N-GDY is expounded by systematical characterizations,especially the synchrotron radiation technique.Doping of F-GDY causes Pb and forms new Pb-F bonds between F-GDY and Pb ions.Doping of N-GDY or GDY brings about Pb(N-GDY doping induces more deviation than that of GDY due to the participation of imine N),improving its electron density and conductivity. | Huan Huang Bing Liu Dan Wang Rongli Cui Xihong Guo Ying Li Shouwei Zuo Zi Yin Huanhua Wang Jing Zhang Hui Yuan Lirong Zheng Baoyun Sun | 2022 | Nano Research2022，15，1： | 2 |
| 3 | Origin of High Efficiency and Long-Term Stability in Ionic Liquid Perovskite Photovoltaic显示文摘Environment-friendly protic amine carboxylic acid ionic liquids(ILs)as solvents is a significant breakthrough with respect to traditional highly coordinating and toxic solvents in achieving efficient and stable perovskite solar cells(PSCs)with a simple one-step air processing and without an antisolvent treatment approach.However,it remains mysterious for the improved efficiency and stability of PSCs without any passivation strategy.Here,we unambiguously demonstrate that the three functions of solvents,additive,and passivation are present for protic amine carboxylic acid ILs.We found that the ILs have the capability to dissolve a series of perovskite precursors,induce oriented crystallization,and chemically passivate the grain boundaries.This is attributed to the unique molecular structure of ILs with carbonyl and amine groups,allowing for strong interaction with perovskite precursors by forming C=O…Pb chelate bonds and N-H…I hydrogen bonds in both solution and film.This finding is generic in nature with extension to a wide range of IL-based perovskite optoelectronics. | Lingfeng Chao Tingting Niu Hao Gu Yingguo Yang Qi Wei Yingdong Xia Wei Hui Shouwei Zuo Zhaohua Zhu Chengjie Pei Xiaodong Li Jing Zhang Junfeng Fang Guichuan Xing Hai Li Xiao Huang Xingyu Gao Chenxin Ran Lin Song Li Fu Yonghua Chen Wei Huang | 2020 | Research2020，，1： | 2 |
| 4 | Ultrahigh Density of Atomic CoFe-Electron Synergy in Noncontinuous Carbon Matrix for Highly Efficient Magnetic Wave Adsorption显示文摘Improving the atom utilization of metals and clarifying the M–M’interaction is both greatly significant in assembling high-performance ultra-light electromagnetic wave-absorbing materials.Herein,a high-temperature explosion strategy has been successfully applied to assemble the hierarchical porous carbon sponge with Co–Fe decoration via the pyrolysis of the energetic metal organic framework.The as-constructed hybrid displays a superior reflection loss(RL)value of-57.7 d B and a specific RL value of-192 d B mg-1 mm-1 at 12.08 GHz with a layer thickness of 2.0 mm(loading of 15 wt%).The off-axis electron hologram characterizes the highly distributed numerous polarized nanodomain variable capacitors,demonstrating the dipole and interfacial polarization along the edges of the nanopores.More importantly,the X-ray absorption spectroscopy analysis verifies the mutual interaction between the metal cluster and carbon matrix and the electronic coupling responsible for the greatly improved electromagnetic wave absorption. | Wenhuan Huang Qiang Qiu Xiufang Yang Shouwei Zuo Jianan Bai Huabin Zhang Ke Pei Renchao Che | 2022 | Nano-Micro Letters2022，14，6： | 1 |
| 5 | Si Doping-Induced Electronic Structure Regulation of Single-Atom Fe Sites for Boosted CO_(2) Electroreduction at Low Overpotentials显示文摘Transition metal-based single-atom catalysts(TM-SACs)are promising alternatives to Au-and Ag-based electrocatalysts for CO production through CO_(2)reduction reaction.However,developing TM-SACs with high activity and selectivity at low overpotentials is challenging.Herein,a novel Fe-based SAC with Si doping(Fe-N-C-Si)was prepared,which shows a record-high electrocatalytic performance toward the CO_(2)-to-CO conversion with exceptional current density(>350.0 mA cm^(−2))and~100%Faradaic efficiency(FE)at the overpotential of<400 mV,far superior to the reported Fe-based SACs.Further assembling Fe-N-C-Si as the cathode in a rechargeable Zn-CO_(2)battery delivers an outstanding performance with a maximal power density of 2.44 mW cm^(−2)at an output voltage of 0.30 V,as well as high cycling stability and FE(>90%)for CO production.Experimental combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulate the electronic structure of the atomic Fe sites in Fe-N-C-Si to markedly accelerate the key pathway involving^(*)CO intermediate desorption,inhibiting the poisoning of the Fe sites under high CO coverage and thus boosting the CO_(2)RR performance.This work provides an efficient strategy to tune the adsorption/desorption behaviors of intermediates on singleatom sites to improve their electrocatalytic performance. | Changsheng Cao Shenghua Zhou Shouwei Zuo Huabin Zhang Bo Chen Junheng Huang Xin-Tao Wu Qiang Xu Qi-Long Zhu | 2023 | Research2023，，4： | 0 |
| 6 | Surface decorated Ni sites for superior photocatalytic hydrogen production显示文摘Precise construction of isolated reactive centers on semiconductors with well-controlled configurations affords a great opportunity to investigate the reaction mechanisms in the photocatalytic process and realize the targeted conversion of solar energy to steer the charge kinetics for hydrogen evolution.In the current research,we decorated isolated Ni atoms on the surface of CdS nanowires for efficient photocatalytic hydrogen production.X-ray absorption fine structure investigations clearly demonstrate the atomical dispersion of Ni sites on the surface of CdS nanowires.Experimental investigations reveal that the isolated Ni atoms not only perform well as the real reactive centers but also greatly accelerate the electron transfer via direct Ni-S coordination.Theoretical simulation further documents that the hydrogen adsorption process has also been enhanced over the semi-coordinated Ni centers through electronic coupling at the atomic scale. | Wenhuan Huang Tingting Bo Shouwei Zuo Yunzhi Wang Jiamin Chen Samy Ould-Chikh Yang Li Wei Zhou Jing Zhang Huabin Zhang | 2022 | SusMat2022，2，4： | 0 |
| 7 | Stable Metal–Halide Perovskite Colloids in Protic Ionic Liquid显示文摘Obtaining long-term stable and robust perovskite colloids solution remains an important scientific challenge due to the limited interaction between solvent and perovskite solutes.Here,we unveil the formation mechanism of chemically robust perovskite precursor solutions under ambient conditions using methylammonium acetate(CH3NH3•CH3COO,MAAc)protic ionic liquid(PIL)solvent.Tens of nanometers colloids are assembled on the molecular level via regular oriented gel-like lamellae with a mean thickness of 34.69 nm,width of 56.81 nm,and distance of 91.05 nm. | Hao Gu Tingting Niu Shouwei Zuo Yongqing Cai Lingfeng Chao Peter Müller-Buschbaum Yingdong Xia Jing Zhang Guichuan Xing Yonghua Chen | 2022 | CCS Chemistry2022，4，10： | 0 |
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