Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin f...Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps process.The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol.The utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up.In the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.展开更多
Tajikistan,a mountainous country and a vital water tower for Central Asia,is becoming increasingly vulnerable to snow drought under climate change,threatening its snow-and glacier-fed streamflow.Yet,the impacts of sno...Tajikistan,a mountainous country and a vital water tower for Central Asia,is becoming increasingly vulnerable to snow drought under climate change,threatening its snow-and glacier-fed streamflow.Yet,the impacts of snow drought on the regional hydrology remain insufficiently understood.In this study,we integrated multisource data,including the Fifth Generation European Centre for Medium-Range Weather Forecasts Atmospheric Reanalysis for Land Applications(ERA5-Land)data and hydrological station data,to systematically assess the snow drought patterns and their impacts on streamflow during 1950–2023.We identified snow drought events based on precipitation and snow fraction anomalies relative to climatological means and classified them into warm snow drought,dry snow drought,and warm&dry snow drought.The results revealed that snow drought was a recurrent phenomenon,occurring in 51.70%of the years during the study period,with warm&dry snow drought accounting for 21.90%of the total events.Both the frequency and severity exhibited pronounced spatial variability,largely governed by the elevation and snowfall fraction.Specifically,the frequency of warm snow drought was negatively correlated with the snowfall fraction,decreasing on average by 0.20 per unit increase in snowfall fraction,whereas the frequency of dry snow drought was positively correlated,increasing by 0.07 per unit increase.The streamflow analysis results demonstrated that snow drought typically reduced the warm-season discharge by 5.00%–18.00%in certain rivers,thereby exacerbating the water stress during the dry season.The results of this study advance our understanding by explicitly linking the types of snow drought to hydrological responses in Central Asia’s high mountains,providing a scientific basis for climate adaptation and sustainable water resource management in Tajikistan.展开更多
Developing advanced electrocatalysts to convert CO_(2) into liquid fuels such as C_(2)H_(5)OH is critical for utilizing intermittent renewable energy.The formation of C_(2)H_(5)OH,however,is generally less favored com...Developing advanced electrocatalysts to convert CO_(2) into liquid fuels such as C_(2)H_(5)OH is critical for utilizing intermittent renewable energy.The formation of C_(2)H_(5)OH,however,is generally less favored compared with the other hydrocarbon products from Cu-based electrocatalysts.In this work,an alkanethiolmodified Cu_(2)O nanowire array(OTT-Cu_(2)O) was constructed with asymmetric Cu sites consisting of paired Cu-O and Cu-S motifs to overcome previous limitations of C_(2)H_(5)OH electrosynthesis via CO_(2)RR pathway.This catalyst achieves a high Faradaic efficiency of 45 % for CO_(2)-to-C_(2)H_(5)OH conversion at 300 m A/cm^(2),representing a more than two-fold enhancement over the Cu_(2)O electrode.Mechanistic investigations reveal that the Cu-S site exhibits distinct C-binding capability that stabilizes key intermediates(^(*)OCH_(2) and ^(*)CO),in contrast to the O-affinitive Cu-O site.The asymmetric S-Cu-O configuration promotes thermodynamically favorable asymmetric C-C coupling between ^(*)CO and ^(*)OCH_(2),forming the critical CO-OCH_(2) intermediate and facilitating C_(2)H_(5)OH production,as opposed to symmetric O-Cu-O sites that mainly generate HCOOH.This work offers an effective strategy for designing multi-active-site catalysts toward highly selective CO_(2) reduction to C_(2)H_(5)OH and provides fundamental insight into the reaction mechanism.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(QNTD202302)National Natural Science Foundation of China(22378024)the Foreign expert program(G2022109001L).
文摘Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps process.The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol.The utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up.In the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.
基金supported by the National Key Research and Development Project of China(2025YFE0103300)the National Natural Science Foundation of China(W2412135)+2 种基金the Natural Science Foundation of Xinjiang Uygur Autonomous Region(2024D01A143,2025D01B165)the China Postdoctoral Science Foundation(GZC20250226)the S&T Innovation and Development Project of Information Institution of Ministry of Emergency Management,China(2024506).
文摘Tajikistan,a mountainous country and a vital water tower for Central Asia,is becoming increasingly vulnerable to snow drought under climate change,threatening its snow-and glacier-fed streamflow.Yet,the impacts of snow drought on the regional hydrology remain insufficiently understood.In this study,we integrated multisource data,including the Fifth Generation European Centre for Medium-Range Weather Forecasts Atmospheric Reanalysis for Land Applications(ERA5-Land)data and hydrological station data,to systematically assess the snow drought patterns and their impacts on streamflow during 1950–2023.We identified snow drought events based on precipitation and snow fraction anomalies relative to climatological means and classified them into warm snow drought,dry snow drought,and warm&dry snow drought.The results revealed that snow drought was a recurrent phenomenon,occurring in 51.70%of the years during the study period,with warm&dry snow drought accounting for 21.90%of the total events.Both the frequency and severity exhibited pronounced spatial variability,largely governed by the elevation and snowfall fraction.Specifically,the frequency of warm snow drought was negatively correlated with the snowfall fraction,decreasing on average by 0.20 per unit increase in snowfall fraction,whereas the frequency of dry snow drought was positively correlated,increasing by 0.07 per unit increase.The streamflow analysis results demonstrated that snow drought typically reduced the warm-season discharge by 5.00%–18.00%in certain rivers,thereby exacerbating the water stress during the dry season.The results of this study advance our understanding by explicitly linking the types of snow drought to hydrological responses in Central Asia’s high mountains,providing a scientific basis for climate adaptation and sustainable water resource management in Tajikistan.
基金financial supports of the National Natural Science Foundation of China (NSFC,Nos.52394202,52476056,and 52301232)the Natural Science Foundation of Chongqing Province (No.2024NSCQ-MSX1109)。
文摘Developing advanced electrocatalysts to convert CO_(2) into liquid fuels such as C_(2)H_(5)OH is critical for utilizing intermittent renewable energy.The formation of C_(2)H_(5)OH,however,is generally less favored compared with the other hydrocarbon products from Cu-based electrocatalysts.In this work,an alkanethiolmodified Cu_(2)O nanowire array(OTT-Cu_(2)O) was constructed with asymmetric Cu sites consisting of paired Cu-O and Cu-S motifs to overcome previous limitations of C_(2)H_(5)OH electrosynthesis via CO_(2)RR pathway.This catalyst achieves a high Faradaic efficiency of 45 % for CO_(2)-to-C_(2)H_(5)OH conversion at 300 m A/cm^(2),representing a more than two-fold enhancement over the Cu_(2)O electrode.Mechanistic investigations reveal that the Cu-S site exhibits distinct C-binding capability that stabilizes key intermediates(^(*)OCH_(2) and ^(*)CO),in contrast to the O-affinitive Cu-O site.The asymmetric S-Cu-O configuration promotes thermodynamically favorable asymmetric C-C coupling between ^(*)CO and ^(*)OCH_(2),forming the critical CO-OCH_(2) intermediate and facilitating C_(2)H_(5)OH production,as opposed to symmetric O-Cu-O sites that mainly generate HCOOH.This work offers an effective strategy for designing multi-active-site catalysts toward highly selective CO_(2) reduction to C_(2)H_(5)OH and provides fundamental insight into the reaction mechanism.
