Cu/ZnO-based catalysts are widely employed for methanol synthesis via CO_(2) hydrogenation.The preparation procedure is sensitive to the particle size and interfacial structure,which are considered as potential active...Cu/ZnO-based catalysts are widely employed for methanol synthesis via CO_(2) hydrogenation.The preparation procedure is sensitive to the particle size and interfacial structure,which are considered as potential active centers influencing the rate of both methanol and CO formation.The particle size and the interaction between Cu and the support materials are influenced by the coprecipitation conditions,let alone that the mechanistic divergence remains unclear.In this work,a series of Cu/ZnO/ZrO_(2) catalysts were prepared via co-precipitation at different pH value and systematically characterized.The structure has been correlated with kinetic results to establish the structure-performance relationship.Kinetic analysis demonstrates that methanol synthesis follows a single-site Langmuir-Hinshelwood(L-H)mechanism,i.e.,Cu serves as the active site where CO_(2) and H_(2) competitively adsorb and react to form methanol.In contrast,CO formation proceeds via a dual-site L-H mechanism,where CO_(2) adsorbs onto ZnO and H_(2) onto Cu,with the reaction occurring at the Cu/ZnO interface.Therefore,for the direct formation of methanol,solely reducing the particle size of Cu would not be beneficial.展开更多
In recent years,numer-ous single-atom catalysts(SACs)have been synthesized to activate persulfate(PS)by a non-radical pathway because of its high se-lectivity,and activity for the cata-lyst.Metal-nitrogen-carbon(M-N_(...In recent years,numer-ous single-atom catalysts(SACs)have been synthesized to activate persulfate(PS)by a non-radical pathway because of its high se-lectivity,and activity for the cata-lyst.Metal-nitrogen-carbon(M-N_(x)-C)has been identified as the key active site in SACs.Although methods for preparing SACs have been extensively reported,a systematic summary of the direct construction of M-N_(x)-C,espe-cially unconventional metal-nitrogen-carbon(UM-N_(x)-C,x≠4),on SACs for PS non-radical activation has still not been reported.The role of the M-N_(x)-C active sites on PS non-radical activation is discussed and methods for the formation of M-N_(x)-C and UM-N_(x)-C active sites in SACs and the effect of catalyst carriers such as carbon nitride(g-C_(3)N_(4)),MOFs,COFs,and other car-bon materials are reviewed.Direct and indirect methods,especially for UM-N_(x)-C active site formation,are also elaborated.Factors affecting the formation of a M-N_(x)-C active site on SACs are also discussed.Prospects for the use of M-N_(x)-C active sites for the non-radical activation of PS by SACs to remove organic contaminants from wastewater are evaluated.展开更多
Objective N6-methyladenosine(m6A),the most prevalent epigenetic modification in eukaryotic RNA,plays a pivotal role in regulating cellular differentiation and developmental processes,with its dysregulation implicated ...Objective N6-methyladenosine(m6A),the most prevalent epigenetic modification in eukaryotic RNA,plays a pivotal role in regulating cellular differentiation and developmental processes,with its dysregulation implicated in diverse pathological conditions.Accurate prediction of m6A sites is critical for elucidating their regulatory mechanisms and informing drug development.However,traditional experimental methods are time-consuming and costly.Although various computational approaches have been proposed,challenges remain in feature learning,predictive accuracy,and generalization.Here,we present m6A-PSRA,a dual-branch residual-network-based predictor that fully exploits RNA sequence information to enhance prediction performance and model generalization.Methods m6A-PSRA adopts a parallel dual-branch network architecture to comprehensively extract RNA sequence features via two independent pathways.The first branch applies one-hot encoding to transform the RNA sequence into a numerical matrix while strictly preserving positional information and sequence continuity.This ensures that the biological context conveyed by nucleotide order is retained.A bidirectional long short-term memory network(BiLSTM)then processes the encoded matrix,capturing both forward and backward dependencies between bases to resolve contextual correlations.The second branch employs a k-mer tokenization strategy(k=3),decomposing the sequence into overlapping 3-mer subsequences to capture local sequence patterns.A pre-trained Doc2vec model maps these subsequences into fixeddimensional vectors,reducing feature dimensionality while extracting latent global semantic information via context learning.Both branches integrate residual networks(ResNet)and a self-attention mechanism:ResNet mitigates vanishing gradients through skip connections,preserving feature integrity,while self-attention adaptively assigns weights to focus on sequence regions most relevant to methylation prediction.This synergy enhances both feature learning and generalization capability.Results Across 11 tissues from humans,mice,and rats,m6A-PSRA consistently outperformed existing methods in accuracy(ACC)and area under the curve(AUC),achieving>90%ACC and>95%AUC in every tissue tested,indicating strong cross-species and cross-tissue adaptability.Validation on independent datasets—including three human cell lines(MOLM1,HEK293,A549)and a long-sequence dataset(m6A_IND,1001 nt)—confirmed stable performance across varied biological contexts and sequence lengths.Ablation studies demonstrated that the dual-branch architecture,residual network,and self-attention mechanism each contribute critically to performance,with their combination reducing interference between pathways.Motif analysis revealed an enrichment of m6A sites in guanine(G)and cytosine(C),consistent with known regulatory patterns,supporting the model’s biological plausibility.Conclusion m6A-PSRA effectively captures RNA sequence features,achieving high prediction accuracy and robust generalization across tissues and species,providing an efficient computational tool for m6A methylation site prediction.展开更多
Lithium metal stands out as an exceptionally promising anode material,boasting an extraordinarily high theoretical capacity and impressive energy density.Despite these advantageous characters,the issues of dendrite fo...Lithium metal stands out as an exceptionally promising anode material,boasting an extraordinarily high theoretical capacity and impressive energy density.Despite these advantageous characters,the issues of dendrite formation and volume expansion of lithium metal anodes lead to performance decay and safety concerns,significantly impeding their advancement towards widespread commercial viability.Herein,a lithium-rich Li-B-In composite anode with abundant lithophilic sites and outstanding structural stability is reported to address the mentioned challenges.The evenly distributed Li-In alloy in the bulk phase of anodes act as mixed ion/electron conductors and nucleation sites,facilitating accelerated Li ions transport dynamics and suppressing lithium dendrite formation.Additionally,these micron-sized Li-In particles in LiB fibers framework can enhance overall structural integrity and provide sufficient interior space to accommodate the volume changes during cycling.The electrochemical performance of Li-B-In composite anode exhibits long-term cyclability,superior rate performance and high-capacity retention.This work confirms that the synergy between a 3 D skeleton and hetero-metallic lithiophilic sites can achieve stable and durable lithium metal anodes,offering innovative insights for the practical deployment of lithium metal batteries.展开更多
淮河是一条对华夏文明具有重大意义的河流。但相较于黄河与长江流域,淮河流域的考古及古环境研究较为滞后。桥头遗址是淮河上游一处以石家河文化为主的重要遗址。本研究通过对桥头遗址区及其临近区域的地层调查和室内样品的测试分析,对...淮河是一条对华夏文明具有重大意义的河流。但相较于黄河与长江流域,淮河流域的考古及古环境研究较为滞后。桥头遗址是淮河上游一处以石家河文化为主的重要遗址。本研究通过对桥头遗址区及其临近区域的地层调查和室内样品的测试分析,对该遗址生成前后的环境变化以及古洪水事件与遗址的存续关系等展开了研究。研究发现:桥头遗址生成前大约在8.1~4.6 ka BP(9.1~5.4 cal.ka BP),遗址所在至少方圆2 km的范围区一直被湖沼所覆盖;4.6 ka BP(5.4 cal.ka BP)以后,温暖湿润的气候、地势较高的湖沼相沉积高地以及紧邻作为遗址水源地的母子河等优越的自然环境,吸引了先民来桥头区域生活;4.0 ka BP的气候异常事件、3.5 ka BP(3.9 cal.ka BP)的气候波动所带来的洪水灾害和3.2 ka BP(3.6 cal.ka BP)的淮河改道等自然环境的频繁变动,使得石家河文化以后的1000年时间内遗址区不适宜人类居住。3 ka BP(3.3 cal.ka BP)之后,桥头遗址所在区域的气温逐渐升高变暖,先人再次在此定居;2.5 ka BP(1.8 cal.ka BP)后,气候的剧烈波动、洪水的频繁泛滥再次威胁到人类在桥头遗址区域生产生活,先人从此地再次迁徙。展开更多
基金supported by Research Grant from China Petroleum and Chemical Corp。
文摘Cu/ZnO-based catalysts are widely employed for methanol synthesis via CO_(2) hydrogenation.The preparation procedure is sensitive to the particle size and interfacial structure,which are considered as potential active centers influencing the rate of both methanol and CO formation.The particle size and the interaction between Cu and the support materials are influenced by the coprecipitation conditions,let alone that the mechanistic divergence remains unclear.In this work,a series of Cu/ZnO/ZrO_(2) catalysts were prepared via co-precipitation at different pH value and systematically characterized.The structure has been correlated with kinetic results to establish the structure-performance relationship.Kinetic analysis demonstrates that methanol synthesis follows a single-site Langmuir-Hinshelwood(L-H)mechanism,i.e.,Cu serves as the active site where CO_(2) and H_(2) competitively adsorb and react to form methanol.In contrast,CO formation proceeds via a dual-site L-H mechanism,where CO_(2) adsorbs onto ZnO and H_(2) onto Cu,with the reaction occurring at the Cu/ZnO interface.Therefore,for the direct formation of methanol,solely reducing the particle size of Cu would not be beneficial.
文摘In recent years,numer-ous single-atom catalysts(SACs)have been synthesized to activate persulfate(PS)by a non-radical pathway because of its high se-lectivity,and activity for the cata-lyst.Metal-nitrogen-carbon(M-N_(x)-C)has been identified as the key active site in SACs.Although methods for preparing SACs have been extensively reported,a systematic summary of the direct construction of M-N_(x)-C,espe-cially unconventional metal-nitrogen-carbon(UM-N_(x)-C,x≠4),on SACs for PS non-radical activation has still not been reported.The role of the M-N_(x)-C active sites on PS non-radical activation is discussed and methods for the formation of M-N_(x)-C and UM-N_(x)-C active sites in SACs and the effect of catalyst carriers such as carbon nitride(g-C_(3)N_(4)),MOFs,COFs,and other car-bon materials are reviewed.Direct and indirect methods,especially for UM-N_(x)-C active site formation,are also elaborated.Factors affecting the formation of a M-N_(x)-C active site on SACs are also discussed.Prospects for the use of M-N_(x)-C active sites for the non-radical activation of PS by SACs to remove organic contaminants from wastewater are evaluated.
基金supported by grants from The National Natural Science Foundation of China(12361104)Yunnan Fundamental Research Projects(202301AT070016,202401AT070036)+2 种基金the Youth Talent Program of Xingdian Talent Support Plan(XDYC-QNRC-2022-0514)the Yunnan Province International Joint Laboratory for Intelligent Integration and Application of Ethnic Multilingualism(202403AP140014)the Open Research Fund of Yunnan Key Laboratory of Statistical Modeling and Data Analysis,Yunnan University(SMDAYB2023004)。
文摘Objective N6-methyladenosine(m6A),the most prevalent epigenetic modification in eukaryotic RNA,plays a pivotal role in regulating cellular differentiation and developmental processes,with its dysregulation implicated in diverse pathological conditions.Accurate prediction of m6A sites is critical for elucidating their regulatory mechanisms and informing drug development.However,traditional experimental methods are time-consuming and costly.Although various computational approaches have been proposed,challenges remain in feature learning,predictive accuracy,and generalization.Here,we present m6A-PSRA,a dual-branch residual-network-based predictor that fully exploits RNA sequence information to enhance prediction performance and model generalization.Methods m6A-PSRA adopts a parallel dual-branch network architecture to comprehensively extract RNA sequence features via two independent pathways.The first branch applies one-hot encoding to transform the RNA sequence into a numerical matrix while strictly preserving positional information and sequence continuity.This ensures that the biological context conveyed by nucleotide order is retained.A bidirectional long short-term memory network(BiLSTM)then processes the encoded matrix,capturing both forward and backward dependencies between bases to resolve contextual correlations.The second branch employs a k-mer tokenization strategy(k=3),decomposing the sequence into overlapping 3-mer subsequences to capture local sequence patterns.A pre-trained Doc2vec model maps these subsequences into fixeddimensional vectors,reducing feature dimensionality while extracting latent global semantic information via context learning.Both branches integrate residual networks(ResNet)and a self-attention mechanism:ResNet mitigates vanishing gradients through skip connections,preserving feature integrity,while self-attention adaptively assigns weights to focus on sequence regions most relevant to methylation prediction.This synergy enhances both feature learning and generalization capability.Results Across 11 tissues from humans,mice,and rats,m6A-PSRA consistently outperformed existing methods in accuracy(ACC)and area under the curve(AUC),achieving>90%ACC and>95%AUC in every tissue tested,indicating strong cross-species and cross-tissue adaptability.Validation on independent datasets—including three human cell lines(MOLM1,HEK293,A549)and a long-sequence dataset(m6A_IND,1001 nt)—confirmed stable performance across varied biological contexts and sequence lengths.Ablation studies demonstrated that the dual-branch architecture,residual network,and self-attention mechanism each contribute critically to performance,with their combination reducing interference between pathways.Motif analysis revealed an enrichment of m6A sites in guanine(G)and cytosine(C),consistent with known regulatory patterns,supporting the model’s biological plausibility.Conclusion m6A-PSRA effectively captures RNA sequence features,achieving high prediction accuracy and robust generalization across tissues and species,providing an efficient computational tool for m6A methylation site prediction.
基金Project(2023YFC3905904)supported by the National Key Research and Development Program,ChinaProject(2220197000221)supported by the Team of Foshan National Hi-Tech Industrial Development Zone Industrialization Entrepreneurial Teams Program,ChinaProject(2024ZZTS0373)supported by the Central South University Graduate Student Autonomous Exploration Innovative Programme,China。
文摘Lithium metal stands out as an exceptionally promising anode material,boasting an extraordinarily high theoretical capacity and impressive energy density.Despite these advantageous characters,the issues of dendrite formation and volume expansion of lithium metal anodes lead to performance decay and safety concerns,significantly impeding their advancement towards widespread commercial viability.Herein,a lithium-rich Li-B-In composite anode with abundant lithophilic sites and outstanding structural stability is reported to address the mentioned challenges.The evenly distributed Li-In alloy in the bulk phase of anodes act as mixed ion/electron conductors and nucleation sites,facilitating accelerated Li ions transport dynamics and suppressing lithium dendrite formation.Additionally,these micron-sized Li-In particles in LiB fibers framework can enhance overall structural integrity and provide sufficient interior space to accommodate the volume changes during cycling.The electrochemical performance of Li-B-In composite anode exhibits long-term cyclability,superior rate performance and high-capacity retention.This work confirms that the synergy between a 3 D skeleton and hetero-metallic lithiophilic sites can achieve stable and durable lithium metal anodes,offering innovative insights for the practical deployment of lithium metal batteries.
文摘淮河是一条对华夏文明具有重大意义的河流。但相较于黄河与长江流域,淮河流域的考古及古环境研究较为滞后。桥头遗址是淮河上游一处以石家河文化为主的重要遗址。本研究通过对桥头遗址区及其临近区域的地层调查和室内样品的测试分析,对该遗址生成前后的环境变化以及古洪水事件与遗址的存续关系等展开了研究。研究发现:桥头遗址生成前大约在8.1~4.6 ka BP(9.1~5.4 cal.ka BP),遗址所在至少方圆2 km的范围区一直被湖沼所覆盖;4.6 ka BP(5.4 cal.ka BP)以后,温暖湿润的气候、地势较高的湖沼相沉积高地以及紧邻作为遗址水源地的母子河等优越的自然环境,吸引了先民来桥头区域生活;4.0 ka BP的气候异常事件、3.5 ka BP(3.9 cal.ka BP)的气候波动所带来的洪水灾害和3.2 ka BP(3.6 cal.ka BP)的淮河改道等自然环境的频繁变动,使得石家河文化以后的1000年时间内遗址区不适宜人类居住。3 ka BP(3.3 cal.ka BP)之后,桥头遗址所在区域的气温逐渐升高变暖,先人再次在此定居;2.5 ka BP(1.8 cal.ka BP)后,气候的剧烈波动、洪水的频繁泛滥再次威胁到人类在桥头遗址区域生产生活,先人从此地再次迁徙。
