Engineering hierarchical quaternary superstructure of an integrated MOF-derived electrode for boosting urea electrooxidation assisted water electrolysis

Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical performance.Herein,a self-supported integrated electrode(NiCo-ZLDH/NF)with a unique hierarchical quaternary superstructure was fabricated through a self-sacrificing template strategy from the metal–organic framework(Co-ZIF-67)nanoplate arrays,which features an intriguing well-defined hierarchy when taking the unit cells of the NiCo-based layered double hydroxide(NiCo-LDH)as the primary structure,the ultrathin LDH nanoneedles as the secondary structure,the mesoscale hollow plates of the LDH nanoneedle arrays as the tertiary structure,and the macroscale three-dimensional frames of the plate arrays as the quaternary structure.Notably,the distinctive structure of NiCo-ZLDH/NF can not only accelerate both mass and charge transfer,but also expose plentiful accessible active sites with high intrinsic activity,endowing it with an excellent electrochemical performance for urea oxidation reaction(UOR).Specially,it only required the low potentials of 1.335,1.368 and 1.388 V to deliver the current densities of 10,100 and 200 mA cm^(-2),respectively,much superior to those for typical NiCo-LDH.Employing NiCo-ZLDH/NF as the bifunctional electrode for both anodic UOR and cathodic HER,an energy-saving electrolysis system was further explored which can greatly reduce the needed voltage of 213 mV to deliver the current density of 100 mA cm^(-2),as compared to the conventional water electrolysis system composed of OER.This work manifests that it is prospective to explore the hierarchically nanostructured electrodes and the innovative electrolytic technologies for high-efficiency electrocatalysis.

Using CONTAM to design ventilation strategy of negative pressure isolation ward considering different height of door gaps

Infectious disease departments in hospitals require pressure gradient to create unidirectional airflow to prevent the spread of contaminants,typically by creating active air infiltration through the difference between supply and exhaust air volumes.The door gap is the channel of air flow between rooms,so its height has an important influence on the pressure difference and infiltration air volume of the room.There is still a lack of research on setting reasonable ventilation strategies according to the different heights of door gaps at different positions in the building.In this study,model of a set of isolation wards was established and analyzed using the multi-zone simulation software CONTAM,and the ventilation strategies with different heights of door gaps were applied to the actual infection diseases department.The results show that in a building with ventilation system divided by functional area,the difference in the height of the door gaps requires different active infiltration air volumes.Pressure fluctuations in the medical and patient corridors are greater than in other rooms.The significance of this study is to understand the active infiltration of air to guide the design and operation of ventilation systems in infectious disease hospitals or building remodeled to isolate close contacts of COVID-19 patients.It is also instructive for the design of pressure gradients in clean workshops,biological laboratories,and other similar buildings.

Controlled synthesis of MOF-derived hollow and yolk–shell nanocages for improved water oxidation and selective ethylene glycol reformation

Delicately designed metal–organic framework(MOF)-derived nanostructured electrocatalysts are essential for improving the reaction kinetics of the oxygen evolution reaction and tuning the selectivity of small organic molecule oxidation reactions.Herein,novel oxalate-modified hollow CoFe-based layered double hydroxide nanocages(h-CoFe-LDH NCs)and yolk–shell ZIF@CoFe-LDH nanocages(ys-ZIF@CoFe-LDH NCs)are developed through an etching–doping reconstruction strategy from a Co-based MOF precursor(ZIF-67).The distinctive nanostructures,along with the incorporation of the secondary metal element and intercalated oxalate groups,enable h-CoFe-LDH NCs and ys-ZIF@CoFe-LDH NCs to expose more active sites with high intrinsic activity.The resultant h-CoFe-LDH NCs exhibit outstanding OER activity with an overpotential of only 278 mV to deliver a current density of 50 mA cm^(-2).Additionally,controlling the reconstruction degree enables the formation of ys-ZIF@CoFe-LDH NCs with a yolk–shell nanocage nanostructure,which show outstanding electrocatalytic performance for the selective ethylene glycol oxidation reaction(EGOR)toward formate,with a Faradaic efficiency of up to 91%.Consequently,a hybrid water electrolysis system integrating the EGOR and the hydrogen evolution reaction using Pt/C||ys-ZIF@CoFe-LDH NCs is explored for energy-saving hydrogen production,requiring a cell voltage 127 mV lower than water electrolysis to achieve a current density of 50 mA cm^(-2).This work demonstrates a feasible way to design advanced MOF-derived electrocatalysts toward enhanced electrocatalytic reactions.

Si Doping-Induced Electronic Structure Regulation of Single-Atom Fe Sites for Boosted CO_(2) Electroreduction at Low Overpotentials

Transition metal-based single-atom catalysts(TM-SACs)are promising alternatives to Au-and Ag-based electrocatalysts for CO production through CO_(2)reduction reaction.However,developing TM-SACs with high activity and selectivity at low overpotentials is challenging.Herein,a novel Fe-based SAC with Si doping(Fe-N-C-Si)was prepared,which shows a record-high electrocatalytic performance toward the CO_(2)-to-CO conversion with exceptional current density(>350.0 mA cm^(−2))and~100%Faradaic efficiency(FE)at the overpotential of<400 mV,far superior to the reported Fe-based SACs.Further assembling Fe-N-C-Si as the cathode in a rechargeable Zn-CO_(2)battery delivers an outstanding performance with a maximal power density of 2.44 mW cm^(−2)at an output voltage of 0.30 V,as well as high cycling stability and FE(>90%)for CO production.Experimental combined with theoretical analysis unraveled that the nearby Si dopants in the form of Si-C/N bonds modulate the electronic structure of the atomic Fe sites in Fe-N-C-Si to markedly accelerate the key pathway involving^(*)CO intermediate desorption,inhibiting the poisoning of the Fe sites under high CO coverage and thus boosting the CO_(2)RR performance.This work provides an efficient strategy to tune the adsorption/desorption behaviors of intermediates on singleatom sites to improve their electrocatalytic performance.

Impact of different human walking patterns on flow and contaminant dispersion in residential kitchens:Dynamic simulation study

The effects of different human walking patterns on contaminant dispersion in residential kitchens were investigated through computational fluid dynamics simulation with the dynamic mesh method.A tracer gas experiment was performed to verify the feasibility and accuracy of the simulation method.Flow characteristics induced by human walking were minutely described,and the transient capture efficiency of the range hood was adopted to assess the impact of human walking quantitatively.Human walking parallel to a counter,human walking parallel to a counter manned by another human,and human walking toward a counter were studied.Results showed that the mutual effect of the wake and thermal plume caused contaminant dispersion and decreased the performance of the range hood as the human subject walked beside the counter.Even a standing person operated ahead the counter,the wake would affect the thermal plume in a certain extent.The decrement of capture efficiency approached 0.5 in the most unfavorable situation.Moreover,the coaction of the positive/negative pressure zone and impinging air jet drew the thermal plume to the human body.The fluctuation of capture efficiency in this condition was moderate relative to that for the human walking pattern beside the counter.This research could provide a comprehensive overview of different human walking patterns and their impact on residential kitchens and thereby facilitate the maintenance of kitchen air quality.

Direct capture efficiency of range hoods in the confined kitchen space

Range hood is a local ventilation device applied widely in residential kitchen for maintaining healthy environment. This study firstly defines the direct capture efficiency (DCE) based on the two-zone model in a confined kitchen space. A mass flux ratio of the secondary captured pollutant to the entrained pollutant from the room zone is proposed for the determination of DCE, where the distribution coefficient is firstly solved, and then its sensitivity analysis on the DCE is carried out. To validate the mass flux ratio and concisely identify the DCE, a virtual purification method that artificially sets the escaped pollutant to zero, is further applied. Compared with the newly developed DCE, the existing indexes, such as contaminant removal efficiency (CRE), total capture efficiency (TCE), fail to differentiate the direct capture from the total capture. Finally, the effects of such factors as makeup airflow pattern, exhaust flow rate, cooking source temperature and the individual occupied/unoccupied on the DCE are fully studied. It is confirmed that different makeup airflow pattern results in distinguished airflow distribution, which makes a significant difference of more than 30% in DCE. Over 50% increase of DCE can be achieved when the exhaust flow rate is increased from 300 to 600 m3/h. About 30% decrease of DCE is observed with the increased cooking source temperature from 100 to 300 °C, and 10% increase of DCE is appeared in the individual occupied case. This reasonable definition and determination of DCE would help to improve the real capture performance of range hoods.

Combining push-pull airflow and top draft hood for local exhaust of tyre vulcanization process

This paper proposes a push-pull airflow combined with a top draft hood to conduct local exhaust in a rubber workshop.Field measurements are carried out to investigate the characteristics of the emission source,while numerical simulation is performed based on the measurement to test the capture efficiency and to further optimize various parameters including push velocity,hood height and exhaust air rate.Compared with the high-hanging hood,the low-hanging hood can effectively capture the pollutant generated by tyre with lower exhaust air rate.The capture efficiency of the low-hanging hood reaches 98.18%with exhaust air rate of 6000 m^(3)/h and push air velocity of 5m/s.The results indicates that the new ventilation appliance can effectively collect the pollutant at a relatively low exhaust rate.

Pressure and flowrate distribution in central exhaust shaft with multiple randomly operating range hoods

Central flues are now commonly adopted in high-rise residential buildings in China for cooking oil fumes(COF)exhaust.Range hoods of all floors are connected to the central shaft,where oil fumes were gathered and exhausted through the outlet at the building roof.As households may cook and use their range hood at random periods,there is great uncertainty of the amount of COF being exhausted.In addition,users can often adjust the exhaust rate of the range hood according to their needs.As a result,thousands of possible operating conditions consisting of distinct combinations of on/off conditions and fan speed occur randomly in the central COF exhaust system,causing the exhaust performance to vary considerably from condition to condition.This work developed a mathematical model for characterizing the operation of the central COF exhaust system in a high-rise residential building as well as its iterative solving method.Full-scale tests coupled with CFD simulation referring to a real 30-floor building were conducted to validate the proposed model.The results show that the model agreed well with the CFD and experimental data under various system operating conditions.Moreover,the Monte-Carlo method was introduced to simulate the random operating characteristics of the system,and a hundred thousand cases corresponding to distinct system operating conditions were sampled and statistically analyzed.

Influence of materials’hygric properties on the hygrothermal performance of internal thermal insulation composite systems

Internal thermal insulation composite system(ITICS)can be an important measure for the energy-saving retrofitting of buildings.However,ITICS may cause harmful effects on the hygrothermal performance of building envelopes.This work investigated the influence of the materials’hygric properties on the hygrothermal perfor-mance of a typical ITICS in different climate conditions in China.Two base wall materials,the traditional concrete and a new type aerated concrete,were tested and compared for their hygric properties firstly.The influence of the hygroscopicity of exterior plasters,the permeability of insulation materials and the climate conditions were then analyzed with WUFI simulations.The hygrothermal performance was evaluated with consideration of the total water content(TWC)of the walls and the moisture flux strength,the relative humidity(RH)and the mould growth risk at the interface between the base wall and the insulation layer(B-I interface).The numerical analysis implies that the TWC of internal insulated walls depends mainly on the hygroscopicity of exterior plaster and the wind-driven rain intensity.The upper limits for the water absorption coefficient of exterior plasters used in Bei-jing,Shanghai and Fuzhou are 1e-9,1e-10,1e-10 m^(2)/s respectively.When such limits are guaranteed,a vapour tight system created by using insulation materials with a large vapour resistance factor or adding a vapour barrier can improve the hygrothermal performance of ITICS,especially for concrete walls in cold climate.