CHEMISTRY OF MATERIALS
·
2017
·
IF 9.466
Kai Tao,Bin Xue,Samuel Frere,Inna Slutsky,Yi Cao,Wei Wang,Ehud Gazit
Artificial photosynthesis shows a promising potential for sustainable supply of nutritional ingredients. While most studies focus on the assembly of the light-sensitive chromophores to 1-D architectures in an artificial photosynthesis system, other supramolecular morphologies, especially bioinspired ones, which may have more efficient light-harvesting properties, have been far less studied. Here, MCpP-FF, a bioinspired building block fabricated by conjugating porphyrin and diphenylalanine, was designed to self-assemble into nanofibers-based multiporous microspheres. The highly organized aromatic moieties result in extensive excitation red-shifts and notable electron transfer, thus leading to a remarkable attenuated fluorescence decay and broad-spectrum light sensitivity of the microspheres. Moreover, the enhanced photoelectron production and transfer capability of the microspheres are demonstrated, making them ideal candidates for sunlight-sensitive antennas in artificial photosynthesis. These properties induce a high turnover frequency of NADH, which can be used to produce bioproducts in biocatalytic reactions. In addition, the direct electron transfer makes external mediators unnecessary, and the insolubility of the microspheres in water allows their easy retrieval for sustainable applications. Our findings demonstrate an alternative to design new platforms for artificial photosynthesis, as well as a new type of bioinspired, supramolecular multiporous materials.
研究领域:
生物化学
·
材料科学
✓ 已验证
DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2014
·Vol. 16
·期 24
·12008-12013
·
IF 4.198
Yan Gao,Linlin Zhang,Xin Ding,Licheng Sun
Photoactive anodes consisting of Ru(bpy)3 type photosensitizer 1 and molecular catalysts 2 and 3 on nanostructured TiO2 have been assembled in functional devices for successful light driven water splitting. From their performance measurements we found that the photoanode TiO2(1 + 3) in which the molecular ruthenium catalyst and the phosphonate anchoring group are linked by a flexible –CH2CH2CH2– chain showed a significantly higher photocurrent density than the photoanode TiO2(1 + 2) with only –CH2– linkage. The possible reasons for the different water splitting performance of otherwise identical devices are discussed.
研究领域:
化学
·
能源科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Remote Sensing
·
2021
·Vol. 13
·期 16
·3311
·
IF 4.848
Alejandro Sánchez de Miguel,Jonathan Bennie,Emma Rosenfeld,Simon Dzurjak,Kevin J. Gaston
The global spread of artificial light is eroding the natural night-time environment. The estimation of the pattern and rate of growth of light pollution on multi-decadal scales has nonetheless proven challenging. Here we show that the power of global satellite observable light emissions increased from 1992 to 2017 by at least 49%. We estimate the hidden impact of the transition to solid-state light-emitting diode (LED) technology, which increases emissions at visible wavelengths undetectable to existing satellite sensors, suggesting that the true increase in radiance in the visible spectrum may be as high as globally 270% and 400% on specific regions. These dynamics vary by region, but there is limited evidence that advances in lighting technology have led to decreased emissions.Keywords:ALAN;artificial light at night;astronomy;DMSP;LEDs;light pollution;melatonin;nocturnal ecology;VIIRS
研究领域:
环境科学
·
生物学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Wang Shuo,Li Chenyang,Qi Yu,Zhang Jiaming,Wang Ningning,Liu Meng,Zhang Boyang,Cai Xuefen,Zhang Hongbo,Wei Su-huai,Ma Guijun,Yang Jingxiu,Chen Shanshan,Zhang Fuxiang
Charge separation of particulate photocatalysts has been considered as the rate-determining step in artificial photocatalysis since the finding of Honda-Fujishima effect, whose efficiency is generally much lower than that of natural photosynthesis. To approach its upper limit, it requires the photoexcited electrons and holes be efficiently transferred to the spatially separated redox reaction sites over a single photocatalyst particle. Herein, it is demonstrated the spatial charge separation among facets of BiVO 4 :Mo can be notably promoted by creating an electron transfer layer. It not only favors electrons to transfer to its surface, but also promotes the built-in electric field intensity of the inter-facet junction by over 10 times. Consequently, the charge separation efficiency of the modified BiVO 4 :Mo with loading of CoFeO x oxidation cocatalyst exceeds 90% at 420 nm, comparable to that of the natural photosynthesis system, over which notably enhanced photocatalytic activities are achieved. Our findings demonstrate the effectiveness of electron transfer layer in intensifying charge separation of particulate photocatalysts.
研究领域:
材料科学
·
光催化技术
·
能源转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-10
·
IF 14.919
Wu Qingyao,Cao Jingjing,Wang Xiao,Liu Yan,Zhao Yajie,Wang Hui,Liu Yang,Huang Hui,Liao Fan,Shao Mingwang,Kang Zhenghui
Artificial photosynthesis of H 2 O 2 from H 2 O and O 2 , as a spotless method, has aroused widespread interest. Up to date, most photocatalysts still suffer from serious salt-deactivated effects with huge consumption of photogenerated charges, which severely limit their wide application. Herein, by using a phenolic condensation approach, carbon dots, organic dye molecule procyanidins and 4-methoxybenzaldehyde are composed into a metal-free photocatalyst for the photosynthetic production of H 2 O 2 in seawater. This catalyst exhibits high photocatalytic ability to produce H 2 O 2 with the yield of 1776 μmol g −1 h −1 ( λ ≥ 420 nm; 34.8 mW cm −2 ) in real seawater, about 4.8 times higher than the pure polymer. Combining with in-situ photoelectrochemical and transient photovoltage analysis, the active site and the catalytic mechanism of this composite catalyst in seawater are also clearly clarified. This work opens up an avenue for a highly efficient and practical, available catalyst for H 2 O 2 photoproduction in real seawater.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2015
·Vol. 17
·期 16
·10726-10736
·
IF 4.493
Huan Lin,Dan Liu,Jinlin Long,Zizhong Zhang,Huaqiang Zhuang,Yi Zheng,Xuxu Wang
The role of polymers in artificial photosystems has been studied in detail. The photosystems were composed of tris(2,2′-bipyridyl) ruthenium(II) chloride as a photosensitizer (PS), colloidal Pt stabilized by polymer as a hydrogen-evolving catalyst and sodium ascorbate as an electron donor, without the addition of a traditional molecular electron mediator. Comprehensive insights into the production of hydrogen on irradiation with visible light were achieved. Several polymers, including neutral polyvinyl pyrrolidone, anionic poly(sodium 4-styrene sulfonate) and poly(acrylic acid) not only stabilized the nanoparticles, but were also effective in the production of hydrogen. Under the optimum conditions, an outstanding apparent quantum efficiency of 12.8% for the evolution of hydrogen was achieved. The formation of self-assembled and spatially separated donor–acceptor complexes via the non-covalent intermolecular interaction between PS and the polymer–Pt was pivotal in the efficient conversion of solar energy to hydrogen fuel. Important details of the photo-induced electron and energy transfer processes in the self-assembled artificial photosystems were determined by nanosecond transient absorption spectrometry and time-resolved fluorescence spectrometry. The initial step in the photo-catalytic production of hydrogen was a reductive quenching of the triplet excited state of the PS by sodium ascorbate, leading to a reduced form of PS, which could then be quickly quenched by the polymer. The rate-determining step was the electron transfer from PS to the catalyst via the polymer bridge.
研究领域:
化学
·
能源科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Xiyuan Zhou,Kaiwen Wang,Yang Wang,Yongyong Cao,Jiaxing Wang,Hanwen Hu,Guo Yang,Jixiang Hou,Peijie Ma,Chunlang Gao,Chaogang Ban,Youyu Duan,Zhen Wei,Xu Zhang,Cong Wang,Kun Zheng
Artificial photosynthesis for high-value hydrogen peroxide (H2O2) through a two-electron reduction reaction is a green and sustainable strategy. However, the development of highly active H2O2 photocatalysts is impeded by severe carrier recombination, ineffective active sites, and low surface reaction efficiency. We developed a dual optimization strategy to load dense Ni nanoparticles onto ultrathin porous graphitic carbon nitride (Ni-UPGCN). In the absence and presence of sacrificial agents, Ni-UPGCN achieved H2O2 production rates of 169 and 4116 μmol g–1 h–1 with AQY (apparent quantum efficiency) at 420 nm of 3.14% and 17.71%. Forming a Schottky junction, the surface-modified Ni nanoparticles broaden the light absorption boundary and facilitate charge separation, which act as active sites, promoting O2 adsorption and reducing the formation energy of *OOH (reaction intermediate). This results in a substantial improvement in both H2O2 generation activity and selectivity. The Schottky junction of dual modulation strategy provides novel insights into the advancement of highly effective photocatalytic agents for the photosynthesis of H2O2.
研究领域:
材料科学
·
光催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Zongyang Li,Yubo Peng,Jianlong Ji,Yuxuan Cheng,Jie Li,Ying Sun,Min Zhao,Xudong Jin,Huayun Du,Yuying Hao
Perovskite microcrystals (PeMCs) show great potential for creating artificial optical synapses due to their low trap state density, high carrier mobility and high thermal stability. However, it is still a challenge to develop a green manufacture for preparing stable PeMCs. Here, we present a facile ice-confined strategy for achieving high-quality CsPbBr3 PeMCs in pure water. In this method, the lecithin protected PeMCs exhibited remarkable stability in polar solvent (water, ethanol, and acetone), which is due to the strong binding ability between lecithin and lead ions of PeMCs. Moreover, the artificial optical synaptic transistors based on CsPbBr3 PeMCs were successfully prepared. The device successfully simulated visual functions by modeling important synaptic features such as excitatory postsynaptic currents, paired-pulse facilitation, spiking-rate-dependent plasticity, spiking-number-dependent plasticity and short-term memory to long-term memory transition. This work provides a new avenue for the synthesis of stable PeMCs and points to a new strategy for highly efficient artificial optical synaptic transistors.
研究领域:
材料科学
·
神经形态工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
TALANTA
·
2024
·
IF 5.6
Jiayuan Shen,Liang Qiao
Artificial photosynthesis by microbe-semiconductor biohybrid systems has been demonstrated as a valuable strategy in providing sustainable energy and in carbon fixation . However, most of the developed biohybrid systems for light harvesting employ heavy metal materials, especially cadmium sulfide (CdS), which normally cause environmental pollution and restrict the widespread of the systems. Herein, we constructed an environmentally friendly biohybirid system based on a typical acetogenic bacteria, Moorella thermoacetica , coupling with a carbon-based semiconductor, graphitic carbon nitride (g-C 3 N 4 ), to realize light-driven carbon fixation . The proposed biohybrid system displayed outstanding acetate productivity with a quantum yield of 2.66 ± 0.43 %. Non-targeted proteomic analysis indicated that the physiological activity of the bacteria was improved, coupling with the non-toxic material. We further proposed the mechanisms of energy generation, electron transfer and CO 2 fixation of the irradiated biohybrid system by proteomic and metabolomic characterization. With the photoelectron generated in g-C 3 N 4 under illumination, CO 2 is finally converted to acetate via the Wood-Ljungdahl pathway (WLP). Other associated pathways were also proved to be activated, providing extra energy or substrates for acetate production. The study reveals that the future focus of the development of biohybrid systems for light harvesting can be on the metal-free biocompatible material, which can activate the expression of the key enzymes involved in the electron transfer and carbon metabolism under light irradiation .
研究领域:
微生物学
·
生物化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Advanced Science
·
2018
·Vol. 5
·期 7
·1800062
·
IF 12.441
Ke-Xin Zhang,Hui Su,Hong-Hui Wang,Jun-Jun Zhang,Shu-Yu Zhao,Weiwei Lei,Xiao Wei,Xin-Hao Li,Jie-Sheng Chen
Heterojunction photocatalysts at present are still suffering from the low charge separation/transfer efficiency due to the poor charge mobility of semiconductor-based photocatalysts. Atomic-scale heterojunction-type photocatalysts are regarded as a promising and effective strategy to overcome the drawbacks of traditional photocatalysts for higher photoenergy conversion efficiencies. Herein, an atomic-scale heterojunction composed of a boron nitride monolayer and graphene (h-BN-C/G) is constructed to significantly shorten the charge transfer path to promote the activation of molecular oxygen for artificial photosynthesis (exemplified with oxidative coupling of amines to imines). As the thinnest heterojunction, h-BN-C/G gives the highest conversion, which is eightfold higher than that of the mechanical mixture of graphene and boron nitride monolayers. h-BN-C/G exhibits a high turnover frequency value (4.0 mmol benzylamine g −1 h −1 ), which is 2.5-fold higher than that of the benchmark metal-free photocatalyst in the literature under even critical conditions.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 17
·5952-5961
·
IF 6.119
Yiping Mo,Chun Wang,Longfei Xiao,Wenxing Chen,Wangyang Lu
Photocatalytic conversion of CO2 into value-added chemicals is considered to be a promising strategy to capture greenhouse gas as well as produce energy. The exploration of efficient and stable photocatalysts is crucial to promote CO2 reduction. Herein, we report the synthesis of a heterogeneous catalyst by integration of iron phthalocyanine (FePc) with g-C3N4via a simple reflux method, in which FePc works as the catalytic center and g-C3N4 acts as the photosensitizer. After 12 h of light irradiation, the CO yield by using the FePc/g-C3N4 catalyst is found to be 1696.96 μmol g−1 and no liquid products are detected. The mechanism for CO2 photoreduction over the FePc/g-C3N4 hybrid catalyst is proposed. To enhance its practicality and portability, we further load the powder catalyst on polyester fibers (PET). The obtained FePc/g-C3N4@PET exhibits high activity for CO2 reduction under both simulated and natural sunlight, with a CO yield of 493.35 μmol g−1 and 490.53 μmol g−1, respectively in 12 h. This work may pave the way to develop an approach for fabricating high-efficient 2D artificial photosynthetic systems for CO2 reduction.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Jiwu Zhao,Lan Xue,Zhenjie Niu,Liang Huang,Yidong Hou,Zizhong Zhang,Rusheng Yuan,Zhengxin Ding,Xianzhi Fu,Xu Lu,Jinlin Long
Sunlight-driven valorization of CO 2 into fuels is a promising solution to renewable energy storage , but the design of an integrated and efficient solar-to-chemical conversion system remains challenging. Herein, an all-solar-driven artificial photosynthetic system (APS) by tailoring photovoltaic-photoelectrochemical cell which can efficiently produce formic acid fuel from CO 2 and H 2 O with bias-free illumination is demonstrated. Guided by density functional theory (DFT) calculations, a BiOI–Bi (BOI–Bi) cathode catalyst is synthesized, which is highly selective for CO 2 to HCOOH conversion, and coupled with a single crystalline argon-treated TiO 2 (TiO 2 -Ar) photoanode, whose valence band edge is beneficial for the oxidation of H 2 O to O 2 . The APS exhibits high product selectivity, robust activity and good durability. A solar-to-HCOOH selectivity of 96.5% is obtained with a HCOOH yield of 108.2 mmol g −1 h −1 under bias-free illumination of AM1.5G. The device can operate stably for at least 12 h. In particular, an apparent photon quantum efficiency of 7.5% and a solar-to-chemical conversion efficiency (η SCC ) of 8.3% are recorded, rivaling all the incumbent precious-metal-free all-solar-driven components for CO 2 -to-HCOOH conversion. This study highlights the potential of BOI-Bi for CO 2 to HCOOH conversion with high selectivity and its integration into APS system to realize carbon-negative solar-to-chemical conversion with industrial relevance.
研究领域:
能源化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）