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| 1 | Oxygen-induced controllable p-type doping in 2D semiconductor transition metal dichalcogenides显示文摘Exposure to oxygen alters the physical and chemical properties of two-dimensional(2D)transition metal dichalcogenides(TMDs).In particular,oxygen in the ambient may influence the device stability of 2D TMDs over time.Engineering the doping of 2D TMDs,especially hole doping is highly desirable towards their device function.Herein,controllable oxygen-induced p-type doping in a range of hexagonal(MoTe2,WSe2,MoSe2 and PtSe2)and pentagonal(PdSe2)2D TMDs are demonstrated.Scanning tunneling microscopy,electrical transport and X-ray photoelectron spectroscopy are used to probe the origin of oxygen-derived hole doping.Three mechanisms are postulated that contribute to the hole doping in 2D TMDs,namely charge transfer from absorbed oxygen molecules,surface oxides,and chalcogen atom substitution.This work provides insights into the doping effects of oxygen,enabling the engineering of 2D TMDs properties for nanoelectronic applications. | Qijie Liang Jian Gou Arramel Qian Zhang Wenjing Zhang Andrew Thye Shen Wee | 2020 | Nano Research2020，13，12： | 4 |
| 2 | 非均相氮配位单原子光催化剂和电催化剂显示文摘随着能源危机和环境问题的日益突出,人们对可再生能源的开发和利用越来越关注.其中,通过能源转换技术,如光催化、电催化或光(电)催化析氢反应、析氧反应、固氮反应和二氧化碳还原反应等,将清洁、丰富的太阳能和电能转化为化学能是解决能源和环境问题的有效策略之一.能源转换技术实现实际应用的关键在于催化剂的活性、稳定性、选择性和成本等,然而目前催化反应大多采用生产成本高的贵金属基催化剂.因此,亟需开发高效、低成本的非贵金属基催化剂来替代贵金属催化剂.单原子催化剂由于可最大限度地利用结构可控、位置明确的金属活性位点,在多相催化中得到了广泛应用.近年来人们发现,通过单个金属原子与氮配位构建的氮配位单原子催化剂表现出有趣的物理、光学和电子性质,其在光催化和电催化领域的应用研究发展迅速.尽管已经有了大量的相关文献报道,但目前有关氮配位单原子催化剂活性位点的内在光催化和电催化性能的调节原理和催化机理的研究尚不充分.本文综述了近年氮配位的单原子催化剂的合成方法和检测技术,总结了氮配位的单原子催化剂在光催化和电催化领域(如光催化或电催化水裂解、二氧化碳还原及固氮等)的应用,结合高角度环形暗场扫描透射电子显微镜、原位红外光谱、原位X射线吸收近边结构谱、第一性原理计算结果以及催化剂在光电催化转化反应中的性能,从单原子配位本征电子结构、活性位点及载体作用等角度,详细讨论了氮配位单原子催化剂真实活性位及作用机制,深度分析了氮原子配位的单原子催化的反应路径与机理,阐明表面活性位点的微观结构特性,进而为开发新型高效单原子光催化剂提供更多的科学依据.最后,总结了目前氮配位单原子光及电催化剂研究面临的机遇与挑战,并对未来发展进行了展望.深度理解催化剂的构效关系,提高金属单原子活性位点含量及本征活性,对催化剂活性中心局域原子和电子结构进行精准设计与构建,将有助于单原子催化剂走出实验室,进而实现实际应用. | 沈荣晨 郝磊 吴永豪 张鹏 Arramel Arramel 李佑稷 李鑫 | 2022 | Chinese Journal of Catalysis2022，43，10： | 1 |
| 3 | Surface molecular doping of all-inorganic perovskite using zethrenes molecules显示文摘We present an optical and photoelectron spectroscopic study to elucidate the interfacial electronic properties of organic-inorganic semiconductor heterojunctions formed in a kinetically blocked heptazethrene triisopropylsilyl ethynylene (HZ-TIPS) and its homologue,octazethrene (OZ-TIPS) on an all-inorganic perovskite cesium lead bromide (CsPbBr3) surface.The photoluminescence behavior of the underlying perovskites upon differing molecular doping conditions was examined.It turns out that the charge transfer dynamics of thermally-evaporated OZ-TIPS molecule exhibited a faster average lifetime than that of the HZ-TIPS case suggesting the importance of the biradical state in the former molecule.An interfacial dipole was formed at the interface due to the competing interaction between the dispersion force of the bulky TIPS-substituent group and the attractive van der Waals interaction at the first few layers.Photoemission spectroscopy of the physisorbed HZ-TIPS shows chemical shifts,which indicates electron transfer from HZ-TIPS molecules to the CsPbBr3 perovskite single crystal.In contrast,the adsorbed OZ-TIPS molecular layer on CsPbBr3 demonstrates the opposite trend indicating a hole transfer process.The average molecular orientation as determined by near edge X-ray absorption fine structure (NEXAFS) suggests that the HZ-TIPS molecular plane is generally lifted with respect to the perovskite surface.We suggest that the nature of the closed-shell electronic ground state of HZ-TIPS could contribute to the formation of interfacial dipole at the molecule/perovskite interface. | Arramel Hu Pan Aozhen Xie Songyan Hou Xinmao Yin Chi Sin Tang Nguyen T.Hoa Muhammad D.Birowosuto Hong Wang Cuong Dang Andrivo Rusydi Andrew T.S.Wee Jishan Wu | 2019 | Nano Research2019，12，1： | 1 |
| 4 | Tailoring the electronic acceptor–donor heterointerface between black phosphorus and Co_(3)O_(4) for boosting oxygen bifunctional electrocatalysis显示文摘Black phosphorus (BP) as an uprising two-dimensional material exhibits attractive potential in the field of electrocatalysis due to the inherent advantages of high carrier mobility and abundant lone pair electrons.However,the exposed active electrons compel BP to be deactivated by oxidative degradation.Herein,the electronic signature of acceptor-donor heterointerfacial interactions between BP and Co_(3)O_(4)is realized via wet ball milling.The preferential migration of active electrons from BP to Co_(3)O_(4)is achieved at the heterointerface since the Fermi level of BP is higher than that of Co_(3)O_(4).Such relative energetic consideration promotes reasonable oxygen electrocatalytic active sites.Moreover,it significantly suppresses the oxidative degradation of BP.Consequently,the resulting Co_(3)O_(4)/BP heterojunction possesses superior oxygen bifunctional electrocatalytic activity than its parent catalysts.Most importantly,this work promotes an efficient route towards BP-based multifunctional catalysts. | Jing Zou Yilun Zou Haitao Wang Wei Wang Pingxiu Wu Arramel Jizhou Jiang Xin Li | 2023 | Chinese Chemical Letters2023，34，2： | 0 |
| 5 | MXenes/CNTs-based hybrids:Fabrications,mechanisms,and modification strategies for energy and environmental applications显示文摘Emerging two-dimensional(2D)layered metal carbide and nitride materials,commonly termed MXenes,are increasingly recognized for their applications across diverse fields such as energy,environment,and catalysis.In the past few years,MXenes/carbon nanotubes(CNTs)-based hybrids have attracted extensive attention as an important catalyst in energy and environmental fields,due to their superior multifunctions and mechanical stability.This review aims to address the fabrication strategies,the identification of the enhancement mechanisms,and recent progress regarding the design and modification of MXenes/CNTs-based hybrids.A myriad of fabrication techniques have been systematically summarized,including mechanical mixing,spray drying,three-dimensional(3D)printing,self-assembly/in-situ growth,freeze drying,templating,hydrothermal methods,chemical vapor deposition(CVD),and rolling.Importantly,the identification of the enhancement mechanisms was thoroughly discussed from the two dimensions of theoretical simulations and in-situ analysis.Moreover,the recent advancements in profound applications of MXenes/CNTs-based hybrids have also been carefully revealed,including energy storage devices,sensors,water purification systems,and microwave absorption.We also underscore anticipated challenges related to their fabrication,structure,underlying mechanisms,modification approaches,and emergent applications.Consequently,this review offers insights into prospective directions and the future trajectory for these promising hybrids.It is expected that this review can inspire new ideas or provide new research methods for future studies. | Jizhou Jiang Fangyi Li Lei Ding Chengxun Zhang Arramel Xin Li | 2024 | Nano Research2024，17，5： | 0 |
| 6 | 基于机器学习和第一性原理计算构建双电子转移通道加速CO_(2)光还原显示文摘光催化还原CO_(2)技术可以将CO_(2)转化为高附加值化学品,在解决日益严重的环境污染和能源危机方面具有巨大潜力.然而,CO_(2)分子较高的C=O键键能(750 kJ mol^(-1))为其活化和还原带来了挑战.因此,构建具有新型电子转移路径的光催化剂具有重要意义.与传统的单电子传输通道相比,层状材料的多电子传输通道在改善载流子传输能力方面具有明显的优势.然而,设计具有合适参数的多电子通道光催化剂模型仍是重要挑战.本文首先采用理论计算预测了具有双电子转移通道、参数匹配的三元异质结BiOBr-Bi-g-C_(3)N_(4);然后,通过机器学习探讨了各种实验参数对双电子传输通道的光催化活性影响的线性规律,优化了实验参数,制备了光催化活性较高的BiOBr-Bi-g-C_(3)N_(4)催化剂;最后,结合第一性原理计算和实验表征结果揭示了其光催化机理.理论计算结果表明,BiOBr-Bi-g-C_(3)N_(4)异质结具有最佳的吉布斯自由能(|ΔG|),有利于光催化H_(2)O解离和CO_(2)还原.实验发现,在300 W Xe灯照射下,CO_(2)还原光催化活性高达43μmol g^(-1)h^(-1).与Bi-BiOBr和Bi-g-C_(3)N_(4)相比,BiOBr-Bi-g-C_(3)N_(4)催化CO_(2)还原:的速率分别提高了约4.7倍和3.1倍.分析新型结构催化剂之所以具有良好的活性,主要有以下三个原因:(1)三者之间匹配的功函数使得BiOBr和g-C_(3)N_(4)纳米片可以与Bi形成肖特基异质结,在光照下,电子从BiOBr和g-C_(3)N_(4)向Bi转移;此外,g-C_(3)N_(4)纳米片与BiOBr具有相似的层间结构和匹配的能级结构,有利于形成Bi-BiOBr和Bi-g-C_(3)N_(4)双电子传输通道,从而实现载流子的有效分离和转移.(2)丰富的Bi活性位点可以抑制光生载流子的随机分布,使其限域在BiOBr与g-C_(3)N_(4)层间;这些载流子在特定的时间尺度上产生了独特的叠加态,优化了CO_(2)还原的多电子反应动力学路径.(3)g-C_(3)N_(4)的引入提高了Bi-BiOBr的太阳光利用率和比表面积.综上所述,本文成功地预测、设计和制备了一种具有双电子传输通道的新型三元异质结BiOBr-Bi-g-C_(3)N_(4)光催化剂,其表现出较高的光催化CO_(2)还原性能.理论计算和实验结果表明,BiOBr和g-C_(3)N_(4)相似的层间结构和匹配的能级结构使得具有不同弛豫时间的电子能够形成相干态;而Bi作为CO_(2)还原的良好活性位点,能够同时提高BiOBr和g-C_(3)N_(4)的载流子转移性能.因此,具有不同寿命的电子可以参与到CO_(2)还原的过程中去.本文可为高性能CO_(2)还原光催化剂的精准预测和合理设计提供实验和理论参考. | 王立晶 杨天一 冯博 许祥雨 申玉莹 李孜涵 Arramel 江吉周 | 2023 | Chinese Journal of Catalysis2023，54，11： | 0 |
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