Browsing by Author "Wu, Jingjie"
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Item Cryo-mediated exfoliation and fracturing of layered materials into 2D quantum dots(AAAS, 2017) Wang, Yan; Liu, Yang; Zhang, Jianfang; Wu, Jingjie; Xu, Hui; Wen, Xiewen; Zhang, Xiang; Tiwary, Chandra Sekhar; Yang, Wei; Vajtai, Robert; Zhang, Yong; Chopra, Nitin; Odeh, Ihab Nizar; Wu, Yucheng; Ajayan, Pulickel M.Atomically thin quantum dots from layered materials promise new science and applications, but their scalable synthesis and separation have been challenging. We demonstrate a universal approach for the preparation of quantum dots from a series of materials, such as graphite, MoS2, WS2, h-BN, TiS2, NbS2, Bi2Se3, MoTe2, Sb2Te3, etc., using a cryo-mediated liquid-phase exfoliation and fracturing process. The method relies on liquid nitrogen pretreatment of bulk layered materials before exfoliation and breakdown into atomically thin two-dimensional quantum dots of few-nanometer lateral dimensions, exhibiting size-confined optical properties. This process is efficient for a variety of common solvents with a wide range of surface tension parameters and eliminates the use of surfactants, resulting in pristine quantum dots without surfactant covering or chemical modification.Item A metal-free electrocatalyst for carbon dioxide reduction to multi-carbon hydrocarbons and oxygenates(Springer Nature, 2016) Wu, Jingjie; Ma, Sichao; Sun, Jing; Gold, Jake I.; Tiwary, ChandraSekhar; Kim, Byoungsu; Zhu, Lingyang; Chopra, Nitin; Odeh, Ihab N.; Vajtai, Robert; Yu, Aaron Z.; Luo, Raymond; Lou, Jun; Ding, Guqiao; Kenis, Paul J.A.; Ajayan, Pulickel M.Electroreduction of carbon dioxide into higher-energy liquid fuels and chemicals is a promising but challenging renewable energy conversion technology. Among the electrocatalysts screened so far for carbon dioxide reduction, which includes metals, alloys, organometallics, layered materials and carbon nanostructures, only copper exhibits selectivity towards formation of hydrocarbons and multi-carbon oxygenates at fairly high efficiencies, whereas most others favour production of carbon monoxide or formate. Here we report that nanometre-size N-doped graphene quantum dots (NGQDs) catalyse the electrochemical reduction of carbon dioxide into multi-carbon hydrocarbons and oxygenates at high Faradaic efficiencies, high current densities and low overpotentials. The NGQDs show a high total Faradaic efficiency of carbon dioxide reduction of up to 90%, with selectivity for ethylene and ethanol conversions reaching 45%. The C2 and C3 product distribution and production rate for NGQD-catalysed carbon dioxide reduction is comparable to those obtained with copper nanoparticle-based electrocatalysts.Item Metallic 1T-TiS2 nanodots anchored on a 2D graphitic C3N4 nanosheet nanostructure with high electron transfer capability for enhanced photocatalytic performance(Royal Society of Chemistry, 2017) Liu, Yang; She, Xiaojie; Zhang, Xiaoni; Liang, Chenglu; Wu, Jingjie; Yu, Peng; Nakanishi, Yusuke; Xie, Banghu; Xu, Hui; Ajayan, Pulickel M.; Yang, WeiPhotocatalysis is one of the most promising technologies for solar energy conversion. With the development of photocatalysis technology, the creation of low-dimensional structure photocatalysts with improved properties becomes more and more important. Metallic 1T-TiS2 nanodots with a low-dimensional structure were introduced into environmentally friendly two-dimensional g-C3N4 (2D-C3N4) nanosheets by a solvothermal method. It was found that the ultrathin TiS2 nanodots were uniformly anchored on the surface of the 2D-C3N4. The effective suppression of electron–hole recombination was realized due to the addition of the intrinsic metallic property of 1T-TiS2 in the prepared nanocomposite. The 5 wt% TiS2/2D-C3N4 nanocomposite exhibited the best photocatalytic performance and the degradation rate towards RhB was ca. 95% in 70 min, which showed an improvement of ca. 30% in comparison with 2D-C3N4. The results indicate that the obtained TiS2/2D-C3N4 nanocomposite is a promising photocatalyst for practical applications.Item Regulation of functional groups on graphene quantum dots directs selective CO2 to CH4 conversion(Springer Nature, 2021) Zhang, Tianyu; Li, Weitao; Huang, Kai; Guo, Huazhang; Li, Zhengyuan; Fang, Yanbo; Yadav, Ram Manohar; Shanov, Vesselin; Ajayan, Pulickel M.; Wang, Liang; Lian, Cheng; Wu, JingjieA catalyst system with dedicated selectivity toward a single hydrocarbon or oxygenate product is essential to enable the industrial application of electrochemical conversion of CO2 to high-value chemicals. Cu is the only known metal catalyst that can convert CO2 to high-order hydrocarbons and oxygenates. However, the Cu-based catalysts suffer from diverse selectivity. Here, we report that the functionalized graphene quantum dots can direct CO2 to CH4 conversion with simultaneous high selectivity and production rate. The electron-donating groups facilitate the yield of CH4 from CO2 electro-reduction while electron-withdrawing groups suppress CO2 electro-reduction. The yield of CH4 on electron-donating group functionalized graphene quantum dots is positively correlated to the electron-donating ability and content of electron-donating group. The graphene quantum dots functionalized by either –OH or –NH2 functional group could achieve Faradaic efficiency of 70.0% for CH4 at −200 mA cm−2 partial current density of CH4. The superior yield of CH4 on electron-donating group- over the electron-withdrawing group-functionalized graphene quantum dots possibly originates from the maintenance of higher charge density of potential active sites (neighboring C or N) and the interaction between the electron-donating group and key intermediates. This work provides insight into the design of active carbon catalysts at the molecular scale for the CO2 electro-reduction.