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La掺杂的TiO_(2)纳米棒在常温常压下可促进电催化的N_(2)转化为NH_(3) 被引量:1
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作者 李莉 陈海军 +12 位作者 李磊 李白海 吴千宝 崔春华 邓彪 罗永岚 刘倩 李廷帅 张芳 abdullah masiri 冯哲圣 王焱 孙旭平 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第10期1755-1762,共8页
氨在化肥、染料、药品和炸药的制造中起着重要作用。目前,传统的Haber-Bosch工艺主要用于NH_(3)的大规模工业化生产,在苛刻的反应条件(300-500℃,150-300 atm)下不可避免地伴随着温室气体的过量排放.因此,必须寻求一种绿色并且可持续的... 氨在化肥、染料、药品和炸药的制造中起着重要作用。目前,传统的Haber-Bosch工艺主要用于NH_(3)的大规模工业化生产,在苛刻的反应条件(300-500℃,150-300 atm)下不可避免地伴随着温室气体的过量排放.因此,必须寻求一种绿色并且可持续的方法来生产NH_(3).电化学还原N_(2)(NRR)已成为在环境条件下将N_(2)连续固定NH_(3)的一种有吸引力的替代方法.由于稳定的N≡N具有较强的偶极矩并与析氢反应存在激烈竞争,因此需要高效的NRR催化剂.TiO_(2)是典型的n型半导体,被认为是一种很有前途的NRR电催化剂.最近的研究表明,La2O3对N_(2)还原电催化也具有活性,然而镧金属的稀土性质限制了其大规模应用.本文研究发现镧可以作为一种有效的掺杂剂提高TiO_(2)的NRR活性.通过水热法制备了镧掺杂的TiO_(2)纳米棒(La-TiO_(2)).透射电子显微镜结果表明,原始TiO_(2)与La-TiO_(2)在形貌上都是纳米棒,镧的引入对其形貌并没有显著影响.选区电子衍射证实了La-TiO_(2)纳米棒的高结晶度和四边形单晶结构.电子自旋共振分析结果表明La-TiO_(2)纳米棒中存在氧空位.La-TiO_(2)的线性扫描伏安曲线结果表明,在N?饱和电解液中的电流密度明显大于在Ar饱和电解液中,说明NRR的发生.为了进一步证实这一假设,在五个不同电位下分别进行了一系列的计时电流测试,结果表明,连续电解2h后在-0.70V时,NH_(3)产率最高,达23.06μg h^(-1) mg_(Cat)^(-1),并且法拉第效率也最大,达14.54%.此外,电解2 h后,没有检测到副产物表明La-TiO_(2)催化剂对NHj合成具有良好的选择性.本文还比较了La-TiO_(2)/CP,TiO_(2)/CP和CP的NRR电催化性能,结果表明,La-TiO_(2)/CP的NH_(3)产率最高,说明La的引入提高了La-TiO_(2)的NRR活性.La-TiO_(2)/CP通过在-0.70V下连续6次循环测试以及连续48 h电解测试证实La-TiO_(2)对NRR电催化具有良好的电化学稳定性.通过对La-O_(v)构型进行密度泛函理论计算,重点研究*N_(2)+H^(+)+e^(-)→*NNH的反应步骤,由于*N_(2)加氢的自由能垒较低,La-TiO_(2)更容易激活N_(2)分子,计算了La-TiO_(2)和纯TiO_(2)上*NNH中间体的电荷密度差异,*NNH与La-TiO_(2)之间存在更多的电荷转移.采用N-N键的积分晶体轨道哈密顿布居(ICOHP)分析出La-TiO_(2)的ICOHP负值较小(-16.67 vs.-19.93),说明N-N键的活化更多. 展开更多
关键词 镧掺杂 电催化氮还原 氧空位 TiO_(2) 密度泛函理论
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Orange-red, green, and blue fiuorescence carbon dots for white light emitting diodes 被引量:2
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作者 Ling Jin Li Zhang +9 位作者 Lei Yang Xingrong Wu Cheng Zhang Kang Wei Lifang He Xinya Han Hongbin Qiao abdullah masiri Khalid AAlamry Kui Zhang 《Journal of Materials Science & Technology》 SCIE EI CAS CSCD 2020年第15期184-191,共8页
Fluorescent carbon dots(CDs) are admirable nanomaterials due to their superior optical properties and low cost.However,regulation of the emission colors in CDs for lighting device still remains a challenge.In this wor... Fluorescent carbon dots(CDs) are admirable nanomaterials due to their superior optical properties and low cost.However,regulation of the emission colors in CDs for lighting device still remains a challenge.In this work,we developed a green hydrothermal method to obtain three emission colors of CDs using L-tyrosine(for blue CDs),o-phenylendiamine(for green CDs) and L-tyrosine/o-phenylendiamine mixture(for orange-red CDs).These CDs possess good water dispersibility,strong emission with high quantum yields,and excellent photostability.Furthermore,the resulting CDs were dispersed in polyvinyl alcohol(PVA) matrix to yield solid state films,where the self-quenching effect in solid state was effectively avoided.A full-color light-emitting diode was fabricated by packing the CDs-PVA composites on the top of a UV-chip,which have superior potential applications in CDs-based solid-state lighting system. 展开更多
关键词 FLUORESCENCE Photoluminescene Carbon dots Self-quenching effect Light-emitting diode
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Highly efficient two-electron electroreduction of oxygen into hydrogen peroxide over Cu-doped TiO_(2)
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作者 Zhiqin Deng Li Li +12 位作者 Yuchun Ren Chaoqun Ma Jie Liang Kai Dong Qian Liu Yonglan Luo Tingshuai Li Bo Tang Yang Liu Shuyan Gao abdullah masiri Shihai Yan Xuping Sun 《Nano Research》 SCIE EI CSCD 2022年第5期3880-3885,共6页
Electrosynthesis of hydrogen peroxide(H2O_(2)),as a sustainable alternative to the anthraquinone oxidation method,provides the feasibility of directly generating H_(2)O_(2).Here,we report Cu-doped TiO_(2) as an effici... Electrosynthesis of hydrogen peroxide(H2O_(2)),as a sustainable alternative to the anthraquinone oxidation method,provides the feasibility of directly generating H_(2)O_(2).Here,we report Cu-doped TiO_(2) as an efficient electrocatalyst which exhibits the excellent two-electron oxygen reduction reaction(2e-ORR)performance with respect to the pristine TiO_(2).The Cu doping results in the distortion of TiO_(2) lattice and further forms a large number of oxygen vacancies and Ti^(3+).Such Cu-doped TiO_(2) exhibits a positive onset potential about 0.79 V and high H_(2)O_(2) selectivity about 91.2%.Moreover,it also shows a larger H_(2)O_(2) yield and good stability.Density functional theory(DFT)calculations reveal that Cu dopant not only improves the electrical conductivity of pristine TiO_(2) but reduces the*OOH adsorption energy of active sites,which is beneficial to promote subsequently 2e-ORR process. 展开更多
关键词 Cu-doped TiO_(2) oxygen vacancy Ti^(3+) two-electron oxygen reduction reaction hydrogen peroxide
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