Shijie YuQinghai LiYanguo ZhangHui Zhou...
163-165页查看更多>>摘要：Plastic waste puts a huge burden on the ecosystem due to the current lack of mature recycling technology.Poly(ethylene terephthalate)(PET)is one of the most produced plastics in the world.Enzymatic decomposition holds the promise of recovering monomers from PET plastic,and the monomers can be used to regenerate new PET products.However,there are still limitations in the activity and thermal stability of the existing PET hydrolases.The recent study by Lu et al.introduced a novel PET hydrolase via machine learning-aided engineering.The obtained PET hydrolase showed excellent activity and thermal stability in the hydrolysis of PET and is capable of directly degrading large amounts of postconsumer PET products.This approach provides an effective method for recycling PET waste and is expected to improve the current state of plastic pollution worldwide.
Xin-Lian SongLei ChenLi-Jiao GaoJin-Tao Ren...
166-197页查看更多>>摘要：Photocatalysis driven by abundant yet intermittent solar energy has considerable potential in renewable energy generation and environmental remediation.The outstanding electronic structure and physicochemical properties of graphitic carbon nitride(g-C3N4),together with unique metal-free characteristic,make them ideal candidates for advanced photocatalysts construction.This review summarizes the up-to-date advances on g-C3N4 based photocatalysts from ingenious-design strategies and diversified photocatalytic applications.Notably,the advantages,fabrication methods and limitations of each design strategy are systemically analyzed.In order to deeply comprehend the inner connection of theory-structure-performance upon g-C3N4 based photocatalysts,structure/composition designs,corresponding photocatalytic activities and reaction mechanisms are jointly discussed,associated with introducing their photocatalytic applications toward water splitting,carbon dioxide/nitrogen reduction and pollutants degradation,etc.Finally,the current challenges and future perspectives for g-C3N4 based materials for photocatalysis are briefly proposed.These design strategies and limitations are also instructive for constructing g-C3N4 based materials in other energy and environment-related applications.
Fukuan LiWeizhe ZhangPeng ZhangAo Gong...
198-216页查看更多>>摘要：Electroreduction of nitrate has been gaining wide attention in recent years owing to it's beneficial for converting nitrate into benign N2 from the perspective of electrocatalytic denitrification or into value-added ammonia from the perspective of electrocatalytic NH3 synthesis.By reason of the undesired formation of ammonia is dominant during electroreduction of nitrate-containing wastewater,chloride has been widely used to improve N2 selectivity.Nevertheless,selective electroreduction of nitrate to N2 gas in chloride-containing system poses several drawbacks.In this review,we focus on the key strategies for efficiently enhancing N2 selectivity of electroreduction of nitrate in chloride-free system,including optimal selection of elements,combining an active metal catalyst with another metal,manipulating the crystalline morphology and facet orientation,constructing core-shell structure catalysts,etc.Before summarizing the strategies,four possible reaction pathways of electro-reduction of nitrate to N2 are discussed.Overall,this review attempts to provide practical strategies for enhancing N2 selectivity without the aid of electrochlorination and highlight directions for future research for designing appropriate electrocatalyst for final electrocatalytic denitrifi-cation.
Yutao LiuLiyu ChenLifeng YangTianhao Lan...
217-310页查看更多>>摘要：Carbon peaking and carbon neutralization trigger a technical revolution in energy & environment related fields.Development of new technologies for green energy production and storage,industrial energy saving and efficiency reinforcement,carbon capture,and pollutant gas treatment is in highly imperious demand.The emerging porous framework materials such as metal-organic frameworks(MOFs),covalent organic frameworks(COFs)and hydrogen-bonded organic frameworks(HOFs),owing to the permanent porosity,tremendous specific surface area,designable structure and customizable functionality,have shown great potential in major energy-consuming industrial processes,including sustainable energy gas catalytic conversion,energy-efficient industrial gas separation and storage.Herein,this manuscript presents a systematic review of porous framework materials for global and comprehensive energy & environment related applications,from a macroscopic and application perspective.
Rui LiQixuan LinJunli RenXiaobao Yang...
311-320页查看更多>>摘要：The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency.Herein,we have developed a simple and effective approach for the selective conversion of fructose to furfural using Hβ zeolite modified by organic acids for dealuminization to regulate its textural and acidic properties.It was found that citric acid-dealuminized Hβ zeolite possessed high specific surface areas,wide channels and high Brønsted acid amount,which facilitated the selective conversion of fructose to furfural with a maximum yield of 76.2％at 433 K for 1 h in the y-butyrolactone(GBL)-H2O system,as well as the concomitant formation of 83.0％formic acid.The 13C-isotope labelling experiments and the mechanism revealed that the selective cleavage of Cl-C2 or C5-C6 bond on fructose was firstly occurred to form pentose or C5 intermediate by weak Brønsted acid,which was then dehydrated to furfural by strong Brønsted acid.Also this dealuminized Hβ catalyst showed the great recycling performance and was active for the conversion of glucose and mannose.
Shaoyu YuanYushan YangZhangyi XiongPeijing Guo...
321-332页查看更多>>摘要：Strong metal-support interaction(SMSI)has a great impact on the activity and selectivity of heterogeneous catalysts,which was usually adjusted by changing reduction temperature or processing catalyst in different atmosphere.However,few researches concentrate on modulating SMSI through regulating the structure of the support.Herein,we show how changing the surface environment of the anatase TiO2(B-TiO2)can be used to modulate the SMSI.The moderate TiOx overlayer makes the Ni metal highly dispersed on the high specific surface area of support,resulting in a substantially enhanced CO2 methanation rate.Besides,a novel phenomenon was observed that boron dopants promote the for-mation of the B-O-Ti interface site,enhancing the catalytic performance of CO2 hydrogenation.DFT calculations confirm that the B-O-Ti structure facilitates the activation of CO2 and further hydrogenation to methane.
Chao WanYu LiangLiu ZhouJindou Huang...
333-343页查看更多>>摘要：The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for chemical hydrogen storage.However,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous challenge.Herein,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution photocatalysts.Impressively,the Co2P nanosheets display extraor-dinary performance with a record high turnover frequency of 44.9 min-1,outperforming most of the noble-metal-free catalysts reported to date.This remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion paths.Our findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.
Yaobin WangQian LuXinlei GeFeng Li...
344-355页查看更多>>摘要：Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO4)group is introduced to modify the surface of PrBa0.5Ca0.5Co2O5+δ(PBCC).The achieved catalyst(PO4-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO4 on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm-2.This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.
Yue ZhangChenlu WangChunlei WangYingyan Zhang...
356-365页查看更多>>摘要：The nanoscale confinement is of great important for the industrial applications of molecular sieve,desalination,and also essential in bio-logical transport systems.Massive efforts have been devoted to the influence of restricted spaces on the properties of confined fluids.However,the situation of channel-wall is crucial but attracts less attention and remains unknown.To fundamentally understand the mechanism of channel-walls in nanoconfinement,we investigated the interaction between the counter-force of the liquid and interlamellar spacing of nanochannel walls by considering the effect of both spatial confinement and surface wettability.The results reveal that the nanochannel stables at only a few discrete spacing states when its confinement is within 1.4 nm.The quantized interlayer spacing is attributed to water molecules becoming laminated structures,and the stable states are corresponding to the monolayer,bilayer and trilayer water configurations,respectively.The results can potentially help to understand the characterized interlayers spacing of graphene oxide membrane in water.Our findings are hold great promise in design of ion filtration membrane and artificial water/ion channels.
Wenmei HanWenli WangJie FanRunping Jia...
366-377页查看更多>>摘要：The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7％+22.8％=57.5％)of the antibacterial efficiency of AZ and gentamicin to 80.2％,net synergizes 22.7％,which fully reflects the effect of 1+1＞2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.
NETL
NSTL
万方数据