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通过调节碳自由基的反应活性调控偶联反应产物和羰基化合物的选择性合成
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作者 陈朝辉 邓军 +3 位作者 郑燕梅 张文君 董琳 陈祖鹏 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第6期135-143,共9页
在温和条件下,生物质(例如,生物质衍生醇、葡萄糖、木糖和木质素)通过光催化转化为高附加值化学品受到了广泛关注.目前,光催化氧化生物质衍生醇的主要产物是羰基化合物,即醛类化合物.相比之下,生物质衍生醇的C–C偶联产物(如氢化苯偶姻... 在温和条件下,生物质(例如,生物质衍生醇、葡萄糖、木糖和木质素)通过光催化转化为高附加值化学品受到了广泛关注.目前,光催化氧化生物质衍生醇的主要产物是羰基化合物,即醛类化合物.相比之下,生物质衍生醇的C–C偶联产物(如氢化苯偶姻和乙二醇)是制药和合成化学领域重要的中间体和原料,具有较大的应用价值.然而,由于对反应机理的理解不足,生物质衍生醇的选择性光催化氧化生成对应的C–C偶联产物和羰基化合物仍然具有挑战性.本文合成了不同金属助催化剂(Au,Pt,Pd和Ru)负载的Cd0.6Zn0.4S复合光催化剂(M-CZS)用于光催化生物质衍生醇的选择性氧化.高分辨透射电镜和X射线光电子能谱结果证明了M-CZS复合光催化剂的成功合成.紫外-可见漫反射光谱结果表明,金属Au和Ru引入后,催化剂可见光的吸收能力增强.采用光致发光光谱、时间分辨光致发光光谱、光电流强度曲线和电化学阻抗曲线研究了催化剂的载流子分离和重组行为,结果表明,金属Au和Ru的引入促进了光生载流子的分离.所制Au-CZS催化剂生成C–C偶联产物(氢化苯偶姻)的速率为40 mmol gcat.^(‒1)h^(‒1),选择性大于98%.Ru-CZS催化剂生成羰基化合物(苯甲醛)的速率为21 mmol gcat.^(‒1)h^(‒1),选择性高达99%.催化剂稳定性测试结果表明,Au-CZS和Ru-CZS催化剂具有良好的光催化稳定性.此外,所制Au-CZS和Ru-CZS催化剂对各种生物质衍生醇具有良好的光催化活性和较高的选择性.电子顺磁共振谱与中间体捕获实验结果表明,反应过程中主要的反应中间体是苯甲醇C_(α)–H键断裂产生的碳自由基中间体.通过密度泛函理论计算研究了Au-CZS和Ru-CZS光催化生物质衍生醇选择性氧化合成偶联产物和羰基化合物过程中,每一步所需的热力学自由能,结果表明,碳自由基中间体在Au和Ru的弱和强吸附,分别导致了C–C偶联产物和羰基化合物的选择性合成.综上,本文报道了一种在Cd0.6Zn0.4S固溶体中引入不同金属助催化剂的策略,通过调节相应碳自由基中间体的反应活性,实现生物质衍生醇的选择性氧化,为生物质衍生醇的高选择性转化提供了新见解. 展开更多
关键词 生物质增值 光催化 碳自由基反应性 选择性控制 吸附能
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Component analysis and risk assessment of biogas slurry from biogas plants 被引量:7
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作者 Lanting Ke Xiaobin Liu +3 位作者 Bingqing Du Yuanpeng Wang yanmei zheng Qingbiao Li 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第4期182-191,共10页
Massive amounts of biogas slurry are produced due to the development of biogas plants.The pollution features and the risk of biogas slurry were fully evaluated in this work.Thirty-one biogas slurry samples were collec... Massive amounts of biogas slurry are produced due to the development of biogas plants.The pollution features and the risk of biogas slurry were fully evaluated in this work.Thirty-one biogas slurry samples were collected from sixteen different cities and five different raw materials biogas plants(e.g.cattle manure,swine manure,straw-manure mixture,kitchen waste and chicken manure).The chemical oxygen demand(COD),ammonia nitrogen(NH_(4)^(+)-N),anions(e.g.Cl^(-1),SO_(4)^(2-),NO_(3)^(-)and PO_(4)^(3-)),antibiotics(e.g.sulphonamides,quinolones,β2-receptor agonists,macrolides,tetracyclines and crystal violet)and heavy metals(e.g.Cu,Cd,As,Cr,Hg,Zn and Pb)contents from these biogas slurry samples were systematically investigated.On this basis,risk assessment of biogas slurry was also performed.The concentrations of COD,NH_(4)^(+)-N and PO_(4)^(3-) in biogas slurry samples with chicken manure as raw material were significantly higher than those of other raw materials.Therefore,the biogas slurry from chicken manure raw material demonstrated the most serious eutrophication threat.The antibiotic contents in biogas slurry samples from swine manure were the highest among five raw materials,mostly sulphonamides,quinolones and tetracyclines.Biogas slurry revealed particularly serious arsenic contamination and moderate potential ecological risk.The quadratic polynomial stepwise regression model can quantitatively describe the correlation among NH_(4)^(+)-N,PO_(4)^(3+) and heavy metals concentration of biogas slurry.This work demonstrated a universal potential threat from biogas slurry that can provide supporting data and theoretical basis for harmless treatment and reuse of biogas slurry. 展开更多
关键词 Biogas slurry ANTIBIOTICS Heavy metals Risk assessment
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稻瘟病菌坏死和乙烯诱导肽1样蛋白的原核表达、纯化与活性分析
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作者 林悦龙 郑燕梅 +5 位作者 王福祥 王颖姮 何炜 蔡秋华 谢华安 张建福 《科学通报》 EI CAS CSCD 北大核心 2023年第7期791-800,共10页
坏死和乙烯诱导肽1(necrosis and ethylene-inducing peptide 1,Nep1)样蛋白(Nep1-like proteins,NLPs)是一类广泛存在于细菌、真菌及卵菌中的分泌型蛋白.本研究通过生物信息学分析了稻瘟病菌中的4个坏死和乙烯诱导肽1样蛋白的家族基因... 坏死和乙烯诱导肽1(necrosis and ethylene-inducing peptide 1,Nep1)样蛋白(Nep1-like proteins,NLPs)是一类广泛存在于细菌、真菌及卵菌中的分泌型蛋白.本研究通过生物信息学分析了稻瘟病菌中的4个坏死和乙烯诱导肽1样蛋白的家族基因成员的相关信息,克隆了它们的编码区序列,分别将它们构建到了pGEX-6P-1载体中.通过优化诱导条件对它们进行了原核表达、纯化,获得了相应的可溶性目的蛋白,进一步将纯化的目的蛋白注射到烟草叶片中,发现N端融合GST标签的MoNLP1、MoNLP4蛋白仍具有生物学活性,可以明显诱发烟草叶片组织产生细胞坏死.该研究为进一步深入研究该基因家族在稻瘟病菌中的功能与作用以及开发更多潜在的植物蛋白激发子奠定基础. 展开更多
关键词 稻瘟病 坏死和乙烯诱导肽1样蛋白 原核表达 蛋白纯化 细胞坏死
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水稻黄绿叶突变体w08(YGL)基因精细定位与功能分析
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作者 蒋家焕 魏林艳 +5 位作者 朱永生 郑燕梅 崔丽丽 蔡秋华 谢华安 张建福 《科学通报》 EI CAS CSCD 北大核心 2022年第30期3580-3594,共15页
水稻黄绿叶突变会显著影响水稻产量和稻米品质.研究黄绿叶突变体叶绿素变化机理对选育高光效品种,促进水稻增产具有重要意义.本研究以甲基磺酸乙酯(ethylmethylsulfone,EMS)诱变处理粳稻云引(YY)后发现的一个黄绿叶突变体w08(YGL)为材料... 水稻黄绿叶突变会显著影响水稻产量和稻米品质.研究黄绿叶突变体叶绿素变化机理对选育高光效品种,促进水稻增产具有重要意义.本研究以甲基磺酸乙酯(ethylmethylsulfone,EMS)诱变处理粳稻云引(YY)后发现的一个黄绿叶突变体w08(YGL)为材料,研究叶色突变对主要农艺性状、叶绿素含量、光合参数变化、水稻生理及亚显微结构的影响,并对该突变性状进行遗传分析、基因定位和功能验证.研究表明,突变体全生育期均表现为黄绿色.与野生型云引(YY)相比,突变体w08单株有效穗、结实率、千粒重分别降低46.7%、50.1%和18.3%,叶绿素a、叶绿素b和类胡萝卜素含量分别下降41.2%、98.7%、17.5%.光合速率检测结果表明,突变体净光合速率(Pn)显著降低,而细胞间CO_(2)(Ci)显著增加.对叶片叶绿体进行超微结构电子显微镜观察,结果发现,叶绿体内的类囊体基粒片层数目在突变体中明显减少.遗传分析结果表明,突变体黄绿叶性状为单基因遗传,受一对隐性核基因控制.利用突变体与雷蒙特(Lemont)杂交构建F2遗传群体,将该基因定位在10号染色体长臂GL8和T258两个标记之间,物理距离为60.2 kb,该区间包含14个候选基因.基因测序发现,该区间内的编码叶绿素酸酯氧化酶1(chlorophyllide a oxygenase1)蛋白的候选基因OsCAO1编码区CDS序列第957位碱基发生突变,形成一个终止密码子,使蛋白翻译提前终止.通过构建过表达和敲除载体进行转基因功能验证,进一步证实了OsCAO1基因功能.分析突变体中的激素含量和分蘖调控相关基因的表达,结果表明,突变体中水稻分蘖相关基因表达水平明显下降,生长素合成基因表达水平显著提高,水稻分蘖芽的生长素含量显著提高,从而证实OsCAO1基因突变抑制了水稻分蘖生长,使单株有效穗显著减少. 展开更多
关键词 水稻 黄绿突变体 基因定位 分蘖 基因表达
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水稻早衰突变体w14的生理学特性分析及其基因的精细定位 被引量:2
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作者 朱永生 蒋家焕 +6 位作者 蔡秋华 郑燕梅 何炜 陈丽萍 魏毅东 王爱荣 张建福 《科学通报》 EI CAS CSCD 北大核心 2021年第32期4144-4156,共13页
水稻叶片早衰对水稻的产量及品质均有重要影响,研究早衰的机理对于延缓衰老和选育良种具有重要意义.本文以甲基磺酸乙酯(ethylmethylsulfone,EMS)诱变野生型粳稻品种云引(Yunyin,YY)获得的水稻早衰突变体w14为材料,研究了早衰突变体全... 水稻叶片早衰对水稻的产量及品质均有重要影响,研究早衰的机理对于延缓衰老和选育良种具有重要意义.本文以甲基磺酸乙酯(ethylmethylsulfone,EMS)诱变野生型粳稻品种云引(Yunyin,YY)获得的水稻早衰突变体w14为材料,研究了早衰突变体全生育期的生理及组织亚显微结构的变化.研究结果表明,突变体从分蘖盛期开始表现出生长势弱,生长速度慢,抽穗期出现明显的叶片早衰症状,最终突变体整株呈现衰老枯萎.亚显微结构观察表明,突变体出现明显衰老表型后,叶片表面泡状细胞破损,细胞结构排列松散,完整性降低,突变体细胞中细胞核数目明显减少,胞内细胞核降解.分别在衰老症状出现前后(苗期和成株期)对突变体和野生型的可溶性蛋白、叶绿素、脂质过氧化物(lipid peroxidation,LPO)及丙二醛(malondialdehyde,MDA)含量和过氧化物酶(peroxidase,POD)、超氧化物歧化酶(superoxide dismutase,SOD)及过氧化氢酶(catalase,CAT)活性进行了系统检测,表明突变体的衰老症状可能主要是由于组织CAT的活性下降导致活性氧(reactive oxygen species,ROS)的累积引起.通过图位克隆方法将目的基因w14定位于水稻3号染色体上,位于InDel标记3-7和3-9之间大约76 kb的物理区间内.该区间内共包含8个候选基因,为该突变性状基因w14的克隆、功能研究和深入了解该突变体早衰的机制奠定了基础. 展开更多
关键词 水稻 早衰 生理特性 显微结构 基因定位
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粳稻云引稻瘟病抗性近等基因系与免疫应答相关的LRR-RLKs差异基因分析 被引量:1
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作者 林悦龙 王昱澎 +8 位作者 朱永生 郑燕梅 蔡秋华 何炜 陈丽萍 谢鸿光 魏毅东 谢华安 张建福 《科学通报》 EI CAS CSCD 北大核心 2021年第30期3873-3885,共13页
在广谱抗稻瘟病品种云引与普感稻瘟病品种丽江新团黑谷(Lijiangxintuanheigu,LTH)构建的近等基因系抗、感病子代基因组重测序的差异基因中,从与免疫应答(immune response)相关的分类单元里得到8个基因序列有差异的基因.它们都为编码富... 在广谱抗稻瘟病品种云引与普感稻瘟病品种丽江新团黑谷(Lijiangxintuanheigu,LTH)构建的近等基因系抗、感病子代基因组重测序的差异基因中,从与免疫应答(immune response)相关的分类单元里得到8个基因序列有差异的基因.它们都为编码富含亮氨酸重复序列的类受体蛋白激酶基因,并聚集于11号染色体的邻近位置,且与已知的白叶枯病抗性基因Xa21具有一定同源性.为进一步探究这些类受体蛋白激酶类基因在稻瘟病抗性中可能发挥的功能,我们分析了这些基因的结构、进化及抗感子代间的序列差异类型,同时还分别采用离体和喷雾接菌的方式对云引和LTH进行稻瘟病接种并取样.通过实时荧光定量PCR(quantitative real time polymerase chain reaction,q RT-PCR)发现,部分基因能受到稻瘟病菌的诱导,推测它们可能在水稻对抗稻瘟病病菌中发挥一定作用,为进一步挖掘稻瘟病相关抗性基因奠定基础. 展开更多
关键词 近等基因系 免疫应答 富含亮氨酸重复序列的类受体蛋白激酶 稻瘟病
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Sulfur-doped g-C3N4/rGO porous nanosheets for highly efficient photocatalytic degradation of refractory contaminants 被引量:4
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作者 yanmei zheng Yuanyuan Liu +6 位作者 Xinli Guo Zhongtao Chen Weijie Zhang Yixuan Wang Xuan Tang Yao Zhang Yuhong Zhao 《Journal of Materials Science & Technology》 SCIE EI CAS CSCD 2020年第6期117-126,共10页
Graphitic carbon nitride(g-C3N4,CN)has attracted increasing interests in the field of photocatalysis due to its high visible-light-response.However,its photocatalytic activity is still lower for degradation of refract... Graphitic carbon nitride(g-C3N4,CN)has attracted increasing interests in the field of photocatalysis due to its high visible-light-response.However,its photocatalytic activity is still lower for degradation of refractory contaminants such as Cr(Ⅵ)and Rhodamine B(RhB)etc.Herein,we report a facile method to synthesize a novel sulfur(S)-doped CN/reduced graphene oxide(rGO)porous nanosheet(S-CN/rGO PNs)via a supramolecular self-assembling followed by a solvothermal treatment.The as-prepared porous SCN/rGO PNs are stable with high specific surface area^188.5 m2 g-1 and exhibit a significantly enhanced photocatalytic activity of^17-fold and 15-fold higher than that of bulk CN for the degradation of RhB and Cr(Ⅵ)under visible light irradiation,respectively.Typically,50 mL of 15 mg/mL RhB can be degraded within 20 min by 10 mg S-CN/rGO PNs.The mechanism can be explained by the synergistic effect of S doping and porous structure which can effectively reduce the band gap of CN and increase the specific surface area to promote the separation and transfer of photo-generated charge carriers.The results have provided a new way to significantly enhance the photocatalytic activity of g-C3N4 for degradation of refractory contaminants. 展开更多
关键词 Sulfur-doped g-C3N4/rGO POROUS nanosheets(S-CN/rGO PNs) Supramolecular self-assembling Solvothermal treatment Photocatalytic activity REFRACTORY CONTAMINANTS
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SH3P2,an SH3 domain-containing protein that interacts with both Pib and AvrPib,suppresses effector-triggered,Pib-mediated immunity in rice 被引量:1
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作者 Yunjie Xie Yupeng Wang +13 位作者 Xiangzhen Yu Yuelong Lin Yongsheng Zhu Jinwen Chen Hongguang Xie Qingqing Zhang Lanning Wang Yidong Wei Yanjia Xiao Qiuhua Cai yanmei zheng Mo Wang Huaan Xie Jianfu Zhang 《Molecular Plant》 SCIE CAS CSCD 2022年第12期1931-1946,共16页
Plants usually keep resistance(R)proteins in a static state under normal conditions to avoid autoimmunity and save energy for growth,but R proteins can be rapidly activated upon perceiving pathogen invasion.Pib,the fi... Plants usually keep resistance(R)proteins in a static state under normal conditions to avoid autoimmunity and save energy for growth,but R proteins can be rapidly activated upon perceiving pathogen invasion.Pib,the first cloned blast disease R gene in rice,encoding a nucleotide-binding leucine-rich repeat(NLR)protein,mediates resistance to the blast fungal(Magnaporthe oryzae)isolates carrying the avirulence gene AvrPib.However,the molecular mechanisms about how Pib recognizes AvrPib and how it is inactivated and activated remain largely unclear.In this study,through map-based cloning and CRISPR-Cas9 gene editing,we proved that Pib contributes to the blast disease resistance of rice cultivar Yunyin(YY).Furthermore,an SH3 domain-containing protein,SH3P2,was found to associate with Pib mainly at clathrin-coated vesicles in rice cells,via direct binding with the coiled-coil(CC)domain of Pib.Interestingly,overexpression of SH3P2 in YY compromised Pib-mediated resistance to M.oryzae isolates carrying AvrPib and Pib-AvrPib recognition-induced cell death.SH3P2 competitively inhibits the self-association of the Pib CC domain in vitro,suggesting that binding of SH3P2 with Pib undermines its homodimerization.Moreover,SH3P2 can also interact with AvrPib and displays higher affinity to AvrPib than to Pib,which leads to dissociation of SH3P2 from Pib in the presence of AvrPib.Taken together,our results suggest that SH3P2 functions as a“protector”to keep Pib in a static state by direct interaction during normal growth but could be triggered off by the invasion of AvrPib-carrying M.oryzae isolates.Our study reveals a new mechanism about how an NLR protein is inactivated under normal conditions but is activated upon pathogen infection. 展开更多
关键词 RICE blast fungus Pib-AvrPib recognition SH3 domain-containing protein PROTECTOR
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Template-free preparation of non-metal(B,P,S)doped g-C_(3)N_(4)tubes with enhanced photocatalytic H_(2)O_(2)generation 被引量:1
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作者 Yuanyuan Liu yanmei zheng +7 位作者 Weijie Zhang zhengbin Peng Hang Xie Yi Xuan Wang Xinli Guo Ming Zhang Rui Li Ying Huang 《Journal of Materials Science & Technology》 SCIE EI CAS CSCD 2021年第36期127-135,共9页
Developing environmentally friendly methods to produce hydrogen peroxide(H_(2)O_(2))has received increasing attention.Photocatalysis has been proved to be a sustainable technology for H_(2)O_(2)production.Herein,the n... Developing environmentally friendly methods to produce hydrogen peroxide(H_(2)O_(2))has received increasing attention.Photocatalysis has been proved to be a sustainable technology for H_(2)O_(2)production.Herein,the novel non-metal elements(B,P,and S)doped g-C_(3)N_(4)tubes(B-CNT,P-CNT,and S-CNT)photocatalysts were obtained via a hydrothermal synthesis followed by thermal polymerization.By adjusting the precursor,the yield of g-C_(3)N_(4)tubes(CNT)materials has been greatly improved.The as-prepared B-CNT,P-CNT,and S-CNT photocatalysts show an enhanced photocatalytic H_(2)O_(2)production with the formation rate constants values of 42.31μM min^(-1),24.95μM min^(-1),and 24.22μM min^(-1),respectively,which is higher than that of bulk CN(16.40μM min^(-1)).The doped B,P,S elements significantly enhanced the photocatalytic activity by adjusting their electronic structures and promoting the separation of electronhole carriers.The results have shown great potential for the practical application of CNT photocatalysts. 展开更多
关键词 Template-free preparation High yield g-C_(3)N_(4)tube(CNT) Non-metal elements doping Photocatalytic H_(2)O_(2)production
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Effects of substrate types on the transformation of heavy metal speciation and bioavailability in an anaerobic digestion system 被引量:1
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作者 Xiarong zheng Kuanhuai Wu +5 位作者 Pengju Sun Siyu Zhouyang Yuanpeng Wang Haitao Wang yanmei zheng Qingbiao Li 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2021年第3期361-372,共12页
Chemical speciation can fundamentally affect the potential toxicity and bioavailability of heavy metals.The transformation of heavy metal speciation and change of bioavailability were investigated in an anaerobic dige... Chemical speciation can fundamentally affect the potential toxicity and bioavailability of heavy metals.The transformation of heavy metal speciation and change of bioavailability were investigated in an anaerobic digestion(AD)system using four different substrates(pig manure(PM),cattle manure(CAM),chicken manure(CHM)and rice straw(RS)).The results obtained indicated that the total contents of heavy metals in PM,CHM and GAM were higher than in RS and decreased in the order Zn>Cu>Ni>Pb>As>Cd in all substrates.Moreover,the speciation with the largest proportion for each heavy metal was the same both in the different substrates and the biogas residues.Among them,Zn,Ni,Cd and As were mainly in the reducible fraction(F2),while Cu was mainly in the oxidizable fraction(F3)and Pb occurred predominantly in the residual fraction(F4).Our results further indicated that the AD process had a greater effect on the speciation of heavy metals in CHM and PM,but less on CAM and RS.The rates of change in bioavailability followed the order PM>CHM>CAM>RS.Changes in organic matter,humic acid or local metal ion environment as a result of AD were inferred as likely mechanisms leading to the transformation of heavy metal speciation.These results enhanced our understanding of the behavior of heavy metals in AD and provided a new perspective for the treatment and disposal of the substrates. 展开更多
关键词 Anaerobic digestion Heavy metal SPECIATION BIOAVAILABILITY
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