The oilseed cake, vetch, rapeseed straw, wheat straw and corn straw were buried in tobacco-planted soil. The decomposition rates, the variation of active organic C and N contents in the residues and the relationship b...The oilseed cake, vetch, rapeseed straw, wheat straw and corn straw were buried in tobacco-planted soil. The decomposition rates, the variation of active organic C and N contents in the residues and the relationship between active organic C and N contents and decomposition rate were investigated. The results showed the decomposition rates of different organic materials were all high in the early period and then low in the late period. Among the organic materials, the decomposition rates ranked as oilseed cake 〉 vetch 〉 wheat straw and rapeseed straw 〉 corn straw. The decomposition rate was positively related to total N content （P〈0.01）, but was negatively related to the active organic C/N ratio （P〈0.01）. However, there was no significant relationship between decomposition ratio and active organic C content. With the proceeding of decomposition, the active organic C content and the total N content in rapeseed straw, vetch, wheat straw and corn straw all trended to increase, but the active organic C/N ratio trended to decrease. However, the variation of active organic C content, total N content and active organic C/N ratio in oilseed cake was on the contrary.展开更多
The use of plant materials as soil amendments is an uncommon practice amongst major farming communities in Ghana, although it is necessary for soil fertility improvement. An examination of the effects of soil amendmen...The use of plant materials as soil amendments is an uncommon practice amongst major farming communities in Ghana, although it is necessary for soil fertility improvement. An examination of the effects of soil amendments is necessary to encourage the use of under-utilized organic resources in Ghana. Thus, a field experiment was conducted using 8 different tropical plant materials mixed with chicken manure as soil amendments for growth of tomato as a test crop. The plant materials included Leucaena leueocephala, Centrosema pubescens, Sesbania sesban, Gliricidia sepium, Mucuna pruriens, Pueraria phaseoloides, Azadirachta indiea, and Theo- broma cacao. There were two other treatments： one with equivalent amounts of chemical fertilizers and the other with no-fertilizer input （control）. Plant materials were mixed with chicken manure to obtain a uniform carbon-to-nitrogen （C：N） ratio of 5：1. Except the no-fertilizer control, all treatments received the same amount of nitrogen （N）. To clarify the decomposition pattern of the plant materials in soil, an incubation experiment was conducted using only the plant materials before the field experiment. The Glirieidia treatment released significantly more mineral N than the other plant materials in the incubation experiment. However, the tomato fruit yield was not enhanced in the Gliricidia treatment in the field experiment. The known quality parameters of the tested plant materials, such as total N, total carbon （C）, C：N ratio, and total polyphenols, had minimal effects on their mineralization dynamics. Azadirachta showed the best synergistic effect with chicken manure through significantly increasing soil microbial biomass and fruit yield of tomato. This result provides insights into the possible adoption of Azadirachta in combination with chicken manure as a soil amendment in small-scale agricultural holdings.展开更多
[目的]为进一步拓展单原子催化剂在亚硝酸盐还原制氨领域的应用,提出了一种铁-氮-碳(Fe-N-C)单原子催化剂电催化亚硝酸盐还原制氨的新体系.[方法]以二氧化硅为硬模板,2,6-二氨基吡啶为碳氮前驱体,硝酸铁为金属盐,通过“热解-刻蚀”策略...[目的]为进一步拓展单原子催化剂在亚硝酸盐还原制氨领域的应用,提出了一种铁-氮-碳(Fe-N-C)单原子催化剂电催化亚硝酸盐还原制氨的新体系.[方法]以二氧化硅为硬模板,2,6-二氨基吡啶为碳氮前驱体,硝酸铁为金属盐,通过“热解-刻蚀”策略制备了Fe-N-C单原子催化剂,并将其应用于亚硝酸盐制氨反应.[结果]多种结构表征结果显示,Fe-N-C催化剂表面的Fe物种呈现高度分散特征并以单原子形式存在.此外,Fe物种的化学环境主要是+2和+3价混合态,且通过与4个吡啶氮配位而稳定存在,即Fe-N-C催化剂的金属中心微观配位环境为Fe-N4结构.与纯氮碳(N-C)载体相比,本研究制备的Fe-N-C催化剂具有优异的亚硝酸盐还原性能,不仅表现出更高的起始还原电位(0 V vs可逆氢电极),具有接近100%的产氨法拉第效率和高的氨产率[8.4 mg/(h·cm^(2))],并且在连续20次催化循环测试中显示出优异的催化稳定性.[结论]本研究制备的Fe-N-C单原子催化剂对亚硝酸盐还原制氨具有优异的电催化活性,其高活性可能来源于对NO_(2)^(-)的显著吸附,并进一步促进活性氢参与脱氧加氢过程.该Fe-N-C单原子催化亚硝酸盐还原体系可为后续合成氨的活性中心设计提供指导方向.展开更多
Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses...Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses challenges to the commercial viability of PEMFCs.Non-platinum group metal(non-PGM)alternatives,like nitrogen-coordinated transition metals in atomic dispersion(M–N–C catalysts),show significant potential.This work presents a comparative study of two distinct sets of Fe–N–C materials,prepared by pyrolyzing hybrid composites of polyaniline(PANI)and iron(Ⅱ)chloride on a hard template.One set uses bipyridine(BPy)as an additional nitrogen source and iron ligand,offering an innovative approach.The findings reveal that the choice of pyrolysis temperature and atmosphere influences the catalyst properties.The use of ammonia in pyrolysis emerges as a crucial parameter for promoting atomic dispersion of iron,as well as increasing surface area and porosity.The optimal catalyst,prepared using BPy and ammonia,exhibits a half-wave potential of 0.834 V in 0.5 M H_(2)SO_(4)(catalyst loading of 0.6 mg cm^(-2)),a mass activity exceeding 3 A g^(-1)and high stability in acidic electrolyte,positioning it as a promising non-PGM structure in the field.展开更多
Environmental catalysis has drawn a great deal ofattention due to its clean ways to produce useful chemicals or carry out some chemical processes.Photocatalysis and electrocatalysis play important roles in these field...Environmental catalysis has drawn a great deal ofattention due to its clean ways to produce useful chemicals or carry out some chemical processes.Photocatalysis and electrocatalysis play important roles in these fields.They can decompose and remove organic pollutants from the aqueous environment,and prepare some fine chemicals.Moreover,they also can carry out some important reactions,such as 02 reduction reaction(ORR),O2 evolution reaction(OER),H2 evolution reaction(HER),CO2 reduction reaction(C02 RR),and N2 fixation(NRR).For catalytic reactions,it is the key to develop high-performance catalysts to meet the demand fortargeted reactions.In recentyears,two-dimensional(2 D) materials have attracted great interest in environmental catalysis due to their unique layered structures,which offer us to make use of their electronic and structural characteristics.Great progress has been made so far,including graphene,black phosphorus,oxides,layered double hydroxides(LDHs),chalcogenides,bismuth-based layered compounds,MXenes,metal organic frameworks(MOFs),covalent organic frameworks(COFs),and others.This content drives us to invite many famous groups in these fields to write the roadmap on two-dimensional nanomaterials for environmental catalysis.We hope that this roadmap can give the useful guidance to researchers in future researches,and provide the research directions.展开更多
The application of electrocatalysts for the oxygen reduction reaction(ORR) is vital in a variety of energy conversion technologies. Exploring low-cost ORR catalysts with high activity and long-term stability is highly...The application of electrocatalysts for the oxygen reduction reaction(ORR) is vital in a variety of energy conversion technologies. Exploring low-cost ORR catalysts with high activity and long-term stability is highly desirable, although it still remains challenging. Herein, we report a facile and reliable route to convert ZIF-8 modified by Fe-phenanthroline into Fe-incorporated and N-doped carbon dodecahedron nanoarchitecture(Fe-NCDNA), in which carbon nanosheets are formed in situ as the building blocks with uniform Fe-N-C species decoration. Systematic electrochemical studies demonstrate that the as-synthesized Fe-NCDNA electrocatalyst possesses highly attractive catalytic features toward the ORR in terms of activity and durability in both alkaline and neutral media. The Zn-air battery with the optimal Fe-NCDNA catalyst as the cathode performs impressively, delivering a power density of 184 m W cm^–2 and a specific capacity of 801 m Ah g^–1;thus, it exhibits great competitive advantages over those of the Zn-air devices employing a Pt-based cathode electrocatalyst.展开更多
A novel coordination polymer, [Fe(C 5H 4NCOO) 2] n, was synthesized by hydrothermal reaction and characterized by elemental analysis as well as IR spectroscopy. The crystal structure (with a novel 3-D network) of this...A novel coordination polymer, [Fe(C 5H 4NCOO) 2] n, was synthesized by hydrothermal reaction and characterized by elemental analysis as well as IR spectroscopy. The crystal structure (with a novel 3-D network) of this compound belongs to monoclinic, space group P2 1/n, a=0.49544(1) nm, b=1.32443(2) nm, c=1.04983(1) nm, β=101.586(1)°. The diffuse reflectance spectra (200～2500 nm) showed that the polymer had strong absorbance in 375～563 nm (E g≈2.5 eV) region and weak absorbance from 720 to 2500 nm (near infrared spectra).展开更多
基金Supported by National Key Technology Research and Development Program(2012BAD40B02Yunnan Provincial Tobacco Company Plan Project(2012YN48)~~
文摘The oilseed cake, vetch, rapeseed straw, wheat straw and corn straw were buried in tobacco-planted soil. The decomposition rates, the variation of active organic C and N contents in the residues and the relationship between active organic C and N contents and decomposition rate were investigated. The results showed the decomposition rates of different organic materials were all high in the early period and then low in the late period. Among the organic materials, the decomposition rates ranked as oilseed cake 〉 vetch 〉 wheat straw and rapeseed straw 〉 corn straw. The decomposition rate was positively related to total N content （P〈0.01）, but was negatively related to the active organic C/N ratio （P〈0.01）. However, there was no significant relationship between decomposition ratio and active organic C content. With the proceeding of decomposition, the active organic C content and the total N content in rapeseed straw, vetch, wheat straw and corn straw all trended to increase, but the active organic C/N ratio trended to decrease. However, the variation of active organic C content, total N content and active organic C/N ratio in oilseed cake was on the contrary.
文摘The use of plant materials as soil amendments is an uncommon practice amongst major farming communities in Ghana, although it is necessary for soil fertility improvement. An examination of the effects of soil amendments is necessary to encourage the use of under-utilized organic resources in Ghana. Thus, a field experiment was conducted using 8 different tropical plant materials mixed with chicken manure as soil amendments for growth of tomato as a test crop. The plant materials included Leucaena leueocephala, Centrosema pubescens, Sesbania sesban, Gliricidia sepium, Mucuna pruriens, Pueraria phaseoloides, Azadirachta indiea, and Theo- broma cacao. There were two other treatments： one with equivalent amounts of chemical fertilizers and the other with no-fertilizer input （control）. Plant materials were mixed with chicken manure to obtain a uniform carbon-to-nitrogen （C：N） ratio of 5：1. Except the no-fertilizer control, all treatments received the same amount of nitrogen （N）. To clarify the decomposition pattern of the plant materials in soil, an incubation experiment was conducted using only the plant materials before the field experiment. The Glirieidia treatment released significantly more mineral N than the other plant materials in the incubation experiment. However, the tomato fruit yield was not enhanced in the Gliricidia treatment in the field experiment. The known quality parameters of the tested plant materials, such as total N, total carbon （C）, C：N ratio, and total polyphenols, had minimal effects on their mineralization dynamics. Azadirachta showed the best synergistic effect with chicken manure through significantly increasing soil microbial biomass and fruit yield of tomato. This result provides insights into the possible adoption of Azadirachta in combination with chicken manure as a soil amendment in small-scale agricultural holdings.
文摘[目的]为进一步拓展单原子催化剂在亚硝酸盐还原制氨领域的应用,提出了一种铁-氮-碳(Fe-N-C)单原子催化剂电催化亚硝酸盐还原制氨的新体系.[方法]以二氧化硅为硬模板,2,6-二氨基吡啶为碳氮前驱体,硝酸铁为金属盐,通过“热解-刻蚀”策略制备了Fe-N-C单原子催化剂,并将其应用于亚硝酸盐制氨反应.[结果]多种结构表征结果显示,Fe-N-C催化剂表面的Fe物种呈现高度分散特征并以单原子形式存在.此外,Fe物种的化学环境主要是+2和+3价混合态,且通过与4个吡啶氮配位而稳定存在,即Fe-N-C催化剂的金属中心微观配位环境为Fe-N4结构.与纯氮碳(N-C)载体相比,本研究制备的Fe-N-C催化剂具有优异的亚硝酸盐还原性能,不仅表现出更高的起始还原电位(0 V vs可逆氢电极),具有接近100%的产氨法拉第效率和高的氨产率[8.4 mg/(h·cm^(2))],并且在连续20次催化循环测试中显示出优异的催化稳定性.[结论]本研究制备的Fe-N-C单原子催化剂对亚硝酸盐还原制氨具有优异的电催化活性,其高活性可能来源于对NO_(2)^(-)的显著吸附,并进一步促进活性氢参与脱氧加氢过程.该Fe-N-C单原子催化亚硝酸盐还原体系可为后续合成氨的活性中心设计提供指导方向.
基金funding from the Hellenic Foundation for Research and Innovation(HFRI)under grant agreement No 3655.
文摘Proton exchange membrane fuel cells(PEMFCs)constitute a promising avenue for environmentally friendly power generation.However,the reliance on unsustainable platinum-based electrocatalysts used at the electrodes poses challenges to the commercial viability of PEMFCs.Non-platinum group metal(non-PGM)alternatives,like nitrogen-coordinated transition metals in atomic dispersion(M–N–C catalysts),show significant potential.This work presents a comparative study of two distinct sets of Fe–N–C materials,prepared by pyrolyzing hybrid composites of polyaniline(PANI)and iron(Ⅱ)chloride on a hard template.One set uses bipyridine(BPy)as an additional nitrogen source and iron ligand,offering an innovative approach.The findings reveal that the choice of pyrolysis temperature and atmosphere influences the catalyst properties.The use of ammonia in pyrolysis emerges as a crucial parameter for promoting atomic dispersion of iron,as well as increasing surface area and porosity.The optimal catalyst,prepared using BPy and ammonia,exhibits a half-wave potential of 0.834 V in 0.5 M H_(2)SO_(4)(catalyst loading of 0.6 mg cm^(-2)),a mass activity exceeding 3 A g^(-1)and high stability in acidic electrolyte,positioning it as a promising non-PGM structure in the field.
基金the National Natural Science Foundation of China (Nos. 21603129 & 20871167)National Natural Science Foundation of Shanxi Province (No. 201601D202021)the Foundation of State Key Laboratory of Coal Conversion (No. J1819-903) for the financial support
文摘Environmental catalysis has drawn a great deal ofattention due to its clean ways to produce useful chemicals or carry out some chemical processes.Photocatalysis and electrocatalysis play important roles in these fields.They can decompose and remove organic pollutants from the aqueous environment,and prepare some fine chemicals.Moreover,they also can carry out some important reactions,such as 02 reduction reaction(ORR),O2 evolution reaction(OER),H2 evolution reaction(HER),CO2 reduction reaction(C02 RR),and N2 fixation(NRR).For catalytic reactions,it is the key to develop high-performance catalysts to meet the demand fortargeted reactions.In recentyears,two-dimensional(2 D) materials have attracted great interest in environmental catalysis due to their unique layered structures,which offer us to make use of their electronic and structural characteristics.Great progress has been made so far,including graphene,black phosphorus,oxides,layered double hydroxides(LDHs),chalcogenides,bismuth-based layered compounds,MXenes,metal organic frameworks(MOFs),covalent organic frameworks(COFs),and others.This content drives us to invite many famous groups in these fields to write the roadmap on two-dimensional nanomaterials for environmental catalysis.We hope that this roadmap can give the useful guidance to researchers in future researches,and provide the research directions.
文摘The application of electrocatalysts for the oxygen reduction reaction(ORR) is vital in a variety of energy conversion technologies. Exploring low-cost ORR catalysts with high activity and long-term stability is highly desirable, although it still remains challenging. Herein, we report a facile and reliable route to convert ZIF-8 modified by Fe-phenanthroline into Fe-incorporated and N-doped carbon dodecahedron nanoarchitecture(Fe-NCDNA), in which carbon nanosheets are formed in situ as the building blocks with uniform Fe-N-C species decoration. Systematic electrochemical studies demonstrate that the as-synthesized Fe-NCDNA electrocatalyst possesses highly attractive catalytic features toward the ORR in terms of activity and durability in both alkaline and neutral media. The Zn-air battery with the optimal Fe-NCDNA catalyst as the cathode performs impressively, delivering a power density of 184 m W cm^–2 and a specific capacity of 801 m Ah g^–1;thus, it exhibits great competitive advantages over those of the Zn-air devices employing a Pt-based cathode electrocatalyst.
文摘研制高活性的Fe/N/C氧还原催化剂对于降低燃料电池成本、实现商业化应用有重要意义.为实现Fe/N/C催化剂的理性设计,需要深入研究其活性位结构.本文发展一种研究活性位结构的新策略,以预先合成好的聚间苯二胺基Fe/N/C催化剂(Pm PDA-Fe Nx/C)为起始物,对其在1000~1500 o C高温下再次进行热处理并使其失活,通过关联催化剂热处理前后的结构变化与氧还原催化性能来揭示活性位结构.实验结果表明,随着热处理温度升高,活性中心结构被破坏,铁原子析出团聚并形成纳米颗粒,氮元素挥发损失,导致催化剂失活.XPS分析显示,低结合能含氮物种的含量与催化剂的ORR活性呈良好的正相关性,表明活性中心很可能是由吡啶N和Fe-N物种构成的.
文摘A novel coordination polymer, [Fe(C 5H 4NCOO) 2] n, was synthesized by hydrothermal reaction and characterized by elemental analysis as well as IR spectroscopy. The crystal structure (with a novel 3-D network) of this compound belongs to monoclinic, space group P2 1/n, a=0.49544(1) nm, b=1.32443(2) nm, c=1.04983(1) nm, β=101.586(1)°. The diffuse reflectance spectra (200～2500 nm) showed that the polymer had strong absorbance in 375～563 nm (E g≈2.5 eV) region and weak absorbance from 720 to 2500 nm (near infrared spectra).
