分类： 生物学 >> 生物物理学 >> 生物物理、生物化学与分子生物学 提交时间： 2016-05-12
摘要： The oxygen-evolving center (OEC) in photosystem II catalyzes a water splitting reaction. Great efforts have already been made to artificially synthesize the OEC, in order to elucidate the structure-function relationship and the mechanism of the reaction. Now, a new synthetic model makes the best mimic yet of the OEC. This recent study opens up the possibility to study the mechanism of photosystem II and photosynthesis in general for applications in renewable energy and synthetic biology.
分类： 生物学 >> 生物物理学 提交时间： 2016-05-12
摘要： Terminal oxidases catalyze four-electron reduction of oxygen to water, and the energy harvested is utilized to drive the synthesis of adenosine triphosphate. While much effort has been made to design a catalyst mimicking the function of terminal oxidases, most biomimetic catalysts have much lower activity than native oxidases. Herein we report a designed oxidase in myoglobin with an O-2 reduction rate (52 s(-1)) comparable to that of a native cytochrome (cyt) cbb(3) oxidase (SO s(-1)) under identical conditions. We achieved this goal by engineering more favorable electrostatic interactions between a functional oxidase model designed in sperm whale myoglobin and its native redox partner, cyt b(5), resulting in a 400-fold electron transfer (ET) rate enhancement. Achieving high activity equivalent to that of native enzymes in a designed metalloenzyme offers deeper insight into the roles of tunable processes such as ET in oxidase activity and enzymatic function and may extend into applications such as more efficient oxygen reduction reaction catalysts for biofuel cells.
分类： 生物学 >> 生态学 提交时间： 2022-06-20 合作期刊: 《干旱区科学》
摘要： Abstract: A knowledge of the tree-ring stable nitrogen isotope ratio (15N) can deepen our understanding of forest ecosystem dynamics by indicating the long-term availability, cycling and sources of nitrogen (N). However, the radial mobility of N blurs the interannual variations in the long-term N records. Previous studies of the chemical extraction of tree rings before analysis had produced inconsistent results and it is still unclear whether it is necessary to pre-treat wood samples from specific tree species to remove soluble N compounds before determining the 15N values. We compared the effects of pre-treatment with organic solvents and hot ultrapure water on the N concentration and 15N of tree rings from endemic Qinghai spruce (Picea crassifolia) growing in the interior of the central Qilian Mountains, China, during the last 60 a. We assessed the effects of different preparation protocols on the removal of the labile N compounds and investigated the need to pre-treat wood samples before determining the 15N values of tree rings. Increasing trends of the tree-ring N concentration were consistently observed in both the extracted and unextracted wood samples. The total N removed by extraction with organic solvents was about 17.60%, with a significantly higher amount in the sapwood section (P<0.01). The 15N values of tree rings decreased consistently from 1960 to 2019 in both the extracted and unextracted wood samples. Extraction with organic solvents increased the 15N values markedly by about 5.2 and reduced the variations in the 15N series. However, extraction with hot ultrapure water had little effect, with only a slight decrease in the 15N values of about 0.5. Our results showed that the radial pattern in the inter-ring movement of N in Qinghai spruce was not minimized by extraction with either organic solvents or hot ultrapure water. It is unnecessary to conduct hot ultrapure water extraction for the wood samples from Qinghai spruce because of its negligible effect on the removal of the labile N. The 15N variation trend of tree rings in the unextracted wood samples was not influenced by the heartwoodsapwood transition zone. We suggest that the 15N values of the unextracted wood samples of the climate-sensitive Qinghai spruce could be used to explore the ecophysiological dynamics while focusing on the long-term variations.
分类： 地球科学 >> 地球科学史 提交时间： 2018-10-29 合作期刊: 《干旱区科学》
XU Guobao
LIU Xiaohong
SUN Weizhen
CHEN Tuo
ZHANG Xuanwen
ZENG Xiaomin
WU Guoju
WANG Wenzhi
QIN Dahe
摘要： Stable isotopes in tree-ring cellulose provide important data in ecological, archaeological, and paleoenvironmental researches, thereby, the demand for stable isotope analyses is increasing rapidly. Simultaneous measurement of cellulose 13C and 18O values from tree rings would reduce the cost of isotopic commodities and improve the analytical efficiency compared with conventional separate measurement. In this study, we compared the 13C and 18O values of tree-ring -cellulose from Tianshan spruce (Picea schrenkiana) in an arid site in the drainage basin of the Urumqi River in Xinjiang of northwestern China based on separate and simultaneous measurements, using the combustion method (at 1050°C) and the high-temperature pyrolysis method (at 1350°C and 1400°C). We verified the results of simultaneous measurement using the outputs from separate measurement and found that both methods (separate and simultaneous) produced similar 13C values. The two-point calibrated method improved the results (range and variation) of 13C and 18O values. The mean values, standard deviations, and trends of the tree-ring 13C obtained by the combustion method were similar to those by the pyrolysis method followed by two-point calibration. The simultaneously measured 18O from the pyrolysis method at 1400°C had a nearly constant offset with that the pyrolysis method at 1350°C due to isotopic-dependence on the reaction temperature. However, they showed similar variations in the time series. The climate responses inferred from simultaneously and separately measured 13C and 18O did not differ between the two methods. The tree-ring 13C and 18O values were negatively correlated with standardized precipitation evapotranspiration index from May to August. In addition, the 18O was significantly correlated with temperature (positive), precipitation (negative), and relative humidity (negative) from May to August. The tree-ring 13C and 18O values determined simultaneously through the high-temperature pyrolysis method could produce acceptable and reliable stable isotope series. The simultaneous isotopic measurement can greatly reduce the cost and time requirement compared with the separate isotopic measurement. These results are consistent with the previous studies at humid sites, suggesting that the simultaneous determination of 13C and 18O in tree-ring -cellulose can be used in wide regions.
分类： 生物学 >> 生物物理学 提交时间： 2016-05-11
Lv, Xiaoxuan
Hu, Cheng
Gao, Feng
Li, Jiasong
Liu, Xiaohong
Deng, Kai
Zheng, Peng
Gong, Weimin
Wang, Jiangyun
Lv, Xiaoxuan
Hu, Cheng
Gao, Feng
Li, Jiasong
Liu, Xiaohong
Deng, Kai
Zheng, Peng
Gong, Weimin
Wang, Jiangyun
Zhou, Meng
Xia, Andong
摘要： Electron transfer (ET) is widely used for driving the processes that underlie the chemistry of life. However, our abilities to probe electron transfer mechanisms in proteins and design redox enzymes are limited, due to :the lack of methods to site-specifically insert electron acceptors into proteins in vivo. Here we describe the synthesis and genetic incorporation of 4-fluoro-3-nitrophenylalanine (FNO(2)Phe), which has similar reduction potentials to NAD(P)H and ferredoxin, the most important biological reductants. Through the genetic incorporation of FNO2Phe into green fluorescent:protein (GFP) and femtosecond transient absorption measurement, we show that photoinduced electron transfer (PET) from the GFP chromophore to FNO2Phe occurs very fast (within 11 ps), which is comparable to that of the first electron transfer step in photosystem I, from P700* to A(0). This genetically encoded, low-reduction potential unnatural amino acid (UAA) can significantly in-Trove our ability to investigate electron transfer mechanisms in complex reductases and facilitate the design of miniature proteins that mimic their functions.
分类： 生物学 >> 生物物理学 提交时间： 2016-05-18
Liu, Xiaohong
Jiang, Li
Li, Jiasong
Wang, Li
Zhou, Qing
Lv, Xiaoxuan
Gong, Weimin
Wang, Jiangyun
Lu, Yi
Lu, Yi
Yu, Yang
摘要： Photo-induced electron transfer (PET) is ubiquitous for photosynthesis and fluorescent sensor design. However, genetically coded PET sensors are underdeveloped, due to the lack of methods to site-specifically install PET probes on proteins. Here we describe a family of acid and Mn(III) turn-on fluorescent protein (FP) sensors, named iLovU, based on PET and the genetic incorporation of superior PET quenchers in the fluorescent flavoprotein iLov. Using the iLovU PET sensors, we monitored the cytoplasmic acidification process, and achieved Mn(III) fluorescence sensing for the first time. The iLovU sensors should be applicable for studying pH changes in living cells, monitoring biogentic Mn(III) in the environment, and screening for efficient manganese peroxidase, which is highly desirable for lignin degradation and biomass conversion. Our work establishes a platform for many more protein PET sensors, facilitates the de novo design of metalloenzymes harboring redox active residues, and expands our ability to probe protein conformational dynamics.
点击量
待评议
点击量
下载量
评论
