Utilization of visible light is of crucial importance for exploiting efficient semiconductor catalysts for solar water splitting. In this study, an advanced ion implantation method was utilized to dope Cu ions into Zn...Utilization of visible light is of crucial importance for exploiting efficient semiconductor catalysts for solar water splitting. In this study, an advanced ion implantation method was utilized to dope Cu ions into ZnO nanorod arrays for photoelectrochemical water splitting in visible light. X-ray diffraction （XRD） and X-ray photo-electron spectroscopy （XPS） results revealed that Cu^＋ together with a small amount of Cu^2＋ were highly dispersed within the ZnO nanorod arrays. The Cu ion doped ZnO nanorod arrays displayed extended optical absorption and enhanced photoelectrochemical performance under visible light illumination （A 〉 420 nm）. A considerable photocurrent density of 18 μA/cm^2 at 0.8 V （vs. a saturated calomel electrode） was achieved, which was about 11 times higher than that of undoped ZnO nanorod arrays. This study proposes that ion implantation could be an effective approach for developing novel visible-light-driven photocatalytic materials for water splitting.展开更多
As the large single-crystalline silicon wafers have revolutionized many industries including electronics and solar cells, it is envisioned that the availability of large single-crystalline perovskite crystals and wafe...As the large single-crystalline silicon wafers have revolutionized many industries including electronics and solar cells, it is envisioned that the availability of large single-crystalline perovskite crystals and wafers will revolutionize its broad applications in photovoltaics, optoelectronics, lasers, photodetectors, light emitting diodes(LEDs), etc. Here we report a method to grow large single-crystalline perovskites including single-halide crystals: CH3NH3PbX3(X=I, Br, Cl), and dual-halide ones:CH3NH3Pb(ClxBr1.x)3 and CH3NH3Pb(BrxI1.x)3, with the largest crystal being 120 mm in length. Meanwhile, we have advanced a process to slice the large perovskite crystals into thin wafers. It is found that the wafers exhibit remarkable features:(1)its trap-state density is a million times smaller than that in the microcrystalline perovskite thin films(MPTF);(2) its carrier mobility is 410 times higher than its most popular organic counterpart P3HT;(3) its optical absorption is expanded to as high as910 nm comparing to 797 nm for the MPTF;(4) while MPTF decomposes at 150 °C, the wafer is stable at high temperature up to270 °C;(5) when exposed to high humidity(75% RH), MPTF decomposes in 5 h while the wafer shows no change for overnight;(6) its photocurrent response is 250 times higher than its MPTF counterpart. A few electronic devices have been fabricated using the crystalline wafers. Among them, the Hall test gives low carrier concentration with high mobility. The trap-state density is measured much lower than common semiconductors. Moreover, the large SC-wafer is found particularly useful for mass production of integrated circuits. By adjusting the halide composition, both the optical absorption and the light emission can be fine-tuned across the entire visible spectrum from 400 nm to 800 nm. It is envisioned that a range of visible lasers and LEDs may be developed using the dual-halide perovskites. With fewer trap states, high mobility, broader absorption, and humidity resistance, it is expected that solar cells with high stable efficiency maybe attainable using the crystalline wafers.展开更多
A series of isomorphic lanthanide coordination polymers [Ln（Ⅲ）（MBP）2（NO3）2（Br）- 2C3H60] [Ln=Eu, Tb, Er, Yb, and Gd; MBP=N,N＇-methylene-bis（pyridin-4-0ne）] featuring polycatenated sql cationic network and i...A series of isomorphic lanthanide coordination polymers [Ln（Ⅲ）（MBP）2（NO3）2（Br）- 2C3H60] [Ln=Eu, Tb, Er, Yb, and Gd; MBP=N,N＇-methylene-bis（pyridin-4-0ne）] featuring polycatenated sql cationic network and incorporated bromide counter ion were prepared. Their visible and near-infrared （NIR） luminescence properties were characterized by steady-state excitation and emission spectra, as well as luminescence lifetimes and quantum yields. The D2d dodecahedron coordination geometry causes visible light excitations and strongly monochromatic emissions. The external heavy-atom environment induces remarkable en- hancement on the NIR emissions. The sensitization processes are revealed by analyzing the electronic properties of MBP ligand.展开更多
A new polymeric nanocomposite photocatalyst A15-CdS with large spherical beads (0.70-0.80 mm in diameter) was fabricated for efficient Rhodamine B (RhB) photodegradation with facile separation during cyclic runs,and p...A new polymeric nanocomposite photocatalyst A15-CdS with large spherical beads (0.70-0.80 mm in diameter) was fabricated for efficient Rhodamine B (RhB) photodegradation with facile separation during cyclic runs,and photocorrosion,a congenital drawback of CdS,was successfully inhibited for A15-CdS.The nanocomposite catalyst was obtained by impregnating CdS nanoparticles within porous polymeric cation exchanger A15 through a facile inner-surface deposition.CdS nanoparticles (<20 nm) immobilized in A15 were deliberately distributed within an outside ring-like region of 40-50 m in depth,which is dominant for photoreaction because visible light is not expected to permeate through the inner region of nontransparent A15.As expected,efficient RhB photodegradation by A15-CdS was achieved under visible light irradiation,and large-size A15-CdS beads are expected to result in their facile separation from solution for repeated use.More significantly,negligible photocorrosion for the hybrid catalyst A15-CdS was demonstrated by the constant photodegradation efficiency and negligible CdS loss during five-cycle runs.The results indicated that nano-CdS immobilization within A15 would greatly improve the applicability of CdS nanoparticles in practical environmental remediation.展开更多
基金The authors gratefully acknowledge the financial support of the National Natural Science Foundation of China （Nos. 51102194, 51323011, and 51121092）, the Doctoral Program of the Ministry of Education （No. 20110201120040） and the Nano Research Program of Suzhou City （ZXG2013003）. S. Shen is supported by the Foundation for the Author of National Excellent Doctoral Dissertation of China （No. 201335） and the Fundamental Research Funds for the Central Universities.
文摘Utilization of visible light is of crucial importance for exploiting efficient semiconductor catalysts for solar water splitting. In this study, an advanced ion implantation method was utilized to dope Cu ions into ZnO nanorod arrays for photoelectrochemical water splitting in visible light. X-ray diffraction （XRD） and X-ray photo-electron spectroscopy （XPS） results revealed that Cu^＋ together with a small amount of Cu^2＋ were highly dispersed within the ZnO nanorod arrays. The Cu ion doped ZnO nanorod arrays displayed extended optical absorption and enhanced photoelectrochemical performance under visible light illumination （A 〉 420 nm）. A considerable photocurrent density of 18 μA/cm^2 at 0.8 V （vs. a saturated calomel electrode） was achieved, which was about 11 times higher than that of undoped ZnO nanorod arrays. This study proposes that ion implantation could be an effective approach for developing novel visible-light-driven photocatalytic materials for water splitting.
基金supported by the National Key Research Project MOST (2016YFA0202400)the National Natural Science Foundation of China (61604090, 61604091, 61674098)+4 种基金National University Research Fund (GK261001009, GK201603107)the Changjiang Scholar and Innovative Research Team (IRT_14R33)the 111 Project (B14041)the Chinese National 1000-talent-plan Program (1110010341)the Innovation Funds of Graduate Programs, SNNU (2015CXS047)
文摘As the large single-crystalline silicon wafers have revolutionized many industries including electronics and solar cells, it is envisioned that the availability of large single-crystalline perovskite crystals and wafers will revolutionize its broad applications in photovoltaics, optoelectronics, lasers, photodetectors, light emitting diodes(LEDs), etc. Here we report a method to grow large single-crystalline perovskites including single-halide crystals: CH3NH3PbX3(X=I, Br, Cl), and dual-halide ones:CH3NH3Pb(ClxBr1.x)3 and CH3NH3Pb(BrxI1.x)3, with the largest crystal being 120 mm in length. Meanwhile, we have advanced a process to slice the large perovskite crystals into thin wafers. It is found that the wafers exhibit remarkable features:(1)its trap-state density is a million times smaller than that in the microcrystalline perovskite thin films(MPTF);(2) its carrier mobility is 410 times higher than its most popular organic counterpart P3HT;(3) its optical absorption is expanded to as high as910 nm comparing to 797 nm for the MPTF;(4) while MPTF decomposes at 150 °C, the wafer is stable at high temperature up to270 °C;(5) when exposed to high humidity(75% RH), MPTF decomposes in 5 h while the wafer shows no change for overnight;(6) its photocurrent response is 250 times higher than its MPTF counterpart. A few electronic devices have been fabricated using the crystalline wafers. Among them, the Hall test gives low carrier concentration with high mobility. The trap-state density is measured much lower than common semiconductors. Moreover, the large SC-wafer is found particularly useful for mass production of integrated circuits. By adjusting the halide composition, both the optical absorption and the light emission can be fine-tuned across the entire visible spectrum from 400 nm to 800 nm. It is envisioned that a range of visible lasers and LEDs may be developed using the dual-halide perovskites. With fewer trap states, high mobility, broader absorption, and humidity resistance, it is expected that solar cells with high stable efficiency maybe attainable using the crystalline wafers.
基金financially supported by the National Natural Science Foundation of China(21431002,91122007)the Specialized Research Fund for the Doctoral Program of Higher Education(20110211130002)
文摘A series of isomorphic lanthanide coordination polymers [Ln（Ⅲ）（MBP）2（NO3）2（Br）- 2C3H60] [Ln=Eu, Tb, Er, Yb, and Gd; MBP=N,N＇-methylene-bis（pyridin-4-0ne）] featuring polycatenated sql cationic network and incorporated bromide counter ion were prepared. Their visible and near-infrared （NIR） luminescence properties were characterized by steady-state excitation and emission spectra, as well as luminescence lifetimes and quantum yields. The D2d dodecahedron coordination geometry causes visible light excitations and strongly monochromatic emissions. The external heavy-atom environment induces remarkable en- hancement on the NIR emissions. The sensitization processes are revealed by analyzing the electronic properties of MBP ligand.
基金support from the National Natural Science Foundation of China (51008151 & 51078179)Jiangsu Natural Science Foundation (BK2009253)+1 种基金the Ministry of Education of China (200802840034)the National High Technology Research and Development Program of China (2009AA06A418)
文摘A new polymeric nanocomposite photocatalyst A15-CdS with large spherical beads (0.70-0.80 mm in diameter) was fabricated for efficient Rhodamine B (RhB) photodegradation with facile separation during cyclic runs,and photocorrosion,a congenital drawback of CdS,was successfully inhibited for A15-CdS.The nanocomposite catalyst was obtained by impregnating CdS nanoparticles within porous polymeric cation exchanger A15 through a facile inner-surface deposition.CdS nanoparticles (<20 nm) immobilized in A15 were deliberately distributed within an outside ring-like region of 40-50 m in depth,which is dominant for photoreaction because visible light is not expected to permeate through the inner region of nontransparent A15.As expected,efficient RhB photodegradation by A15-CdS was achieved under visible light irradiation,and large-size A15-CdS beads are expected to result in their facile separation from solution for repeated use.More significantly,negligible photocorrosion for the hybrid catalyst A15-CdS was demonstrated by the constant photodegradation efficiency and negligible CdS loss during five-cycle runs.The results indicated that nano-CdS immobilization within A15 would greatly improve the applicability of CdS nanoparticles in practical environmental remediation.
