Liwu Zhang

• Principal Investigator at Fudan University

Electrocatalytic reduction of CO2 to formate (HCOO⁻) using Bi‐based nanocatalysts shows great promise in “carbon‐neutrality” and green chemical synthesis. However, the functional active species, metallic Bi or Bi‐O structure responsible for CO2 reduction to HCOO⁻ is still in debate. In this study, we found that nanodendritic Bi‐metal electrocatalys...

Human uptake of microplastic particles (MPs) is causing increasing health concerns, and there is mounting pressure to evaluate the associated risks. While MPs can be ingested, breathed in, or drank in, a very direct entrance channel is available through ingress into the bloodstream. Intravenous infusion usually proceeds from plastic bottles. Many a...

Carbonate radical anion (CO3.-) is generally considered as a marginal intermediate that rarely regulates atmospheric-relevant reactions of significance. Unexpectedly, in this work, employing a suit of the in-field measurements, lab-based validations, improved kinetic numerical calculations, and chemical transport modeling, we demonstrate that CO3.-...

Chirality conferral is fundamental for understanding the origin of life, and it is of direct importance for synthesizing new pharmaceuticals in the face of growing antibiotic resistance. Human-made, self-assembling nanostructures replicate the biological chirality conferral processes utilizing covalent and non-covalent bonds. However, chirality con...

People of all ages consume salt every day, but is it really just salt? Plastic nanoparticles [nanoplastics (NPs)] pose an increasing environmental threat and have begun to contaminate everyday salt in consumer goods. Herein, we developed a combined surface enhanced Raman scattering (SERS) and stimulated Raman scattering (SRS) approach that can real...

The multiphase oxidation of sulfur dioxide (SO2) to form sulfate is a complex and important process in the atmosphere. While the conventional photosensitized reaction mainly explored in the bulk medium is reported to be one of the drivers to trigger atmospheric sulfate production, how this scheme functionalizes at the air–water interface (AWI) of a...

Bioaerosols pose a great threat to human life and health, and developing highly efficient and accurate identification and analysis methodologies for bioaerosols provides prerequisite knowledge to evaluate their toxicity on human health. In this paper, a rapid and economical method is proposed for the detection of bioaerosols based on surface-enhanc...

The negative effects of air pollution, especially fine particulate matter (PM2.5, particles with an aerodynamic diameter of ≤2.5 μm), on human health, climate, and ecosystems are causing significant concern. Nevertheless, little is known about the contributions of emerging pollutants such as plastic particles to PM2.5 due to the lack of continuous...

Carbonate radical anion (CO3.− ${\mathrm{C}{\mathrm{O}}_{3}}^{.-}$) is generally overlooked in atmospheric chemistry. Our recent work emphasizes the important role of carbonate radicals produced on mineral dust surfaces in fast sulfate production under solar irradiation in the presence of CO2 at specifically low RH and light intensity. Yet so far h...

The origin of life on Earth is an enigmatic and intricate conundrum that has yet to be comprehensively resolved despite recent significant developments within the discipline of archaeology and geology. Chemically, metal-sulfide minerals are speculated to serve as an important medium for giving birth in early life while yet so far direct evidence to...

Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Here, we generated dust aerosols from soils to determine if there is particle-size-dependent selectivity of heavy metals in the dust generation. Mn, Cd, Pb and other h...

Severe haze in Beijing is characterized by the rapid formation of sulfate via the multiphase oxidation of SO2. While many factors, including aerosol oxidants and atmospheric variables, were discovered and investigated, their relative importance remains unclear. Herein, based on the field observation data obtained in Beijing, China, we developed a k...

How tiny aqueous aerosol droplets significantly accelerate the atmospheric multiphase reaction remains an open question. Here, we show both experimental and theoretical evidence that the strong electric field at the air/water interface of aerosol particles can be an important driving force to contribute to the fast oxidation of SO2-forming sulfate....

Single-atom catalysts (SACs), as a newcomer in the field of nanocatalysis, have gained intensive interest due to their excellent activities. In this study, single bismuth (Bi) atom-decorated TiO2 catalysts (N-Bi/TiO2) are synthesized by the simple UV irradiation method using Bi(NO3)3 as the precursor. Characterizations confirmed that single Bi atom...

The photocatalytic carbon dioxide reduction reaction (CO2RR) process is one of the most attractive approaches to mitigate the energy crisis by producing a series of fuels such as methane, methanol, formic acid, acetic acid, etc. Unfortunately, these organic products sometimes happen to be the impurity residuals left on photocatalyst surfaces during...

The increasing prevalence of nanoplastics in the environment underscores the need for effective detection and monitoring techniques. Current methods mainly focus on microplastics, while accurate identification of nanoplastics is challenging due to their small size and complex composition. In this work, we combined highly reflective substrates and m...

Solar‐driven CO2 reduction reaction (CO2RR) is largely constrained by the sluggish mass transfer and fast combination of photogenerated charge carriers. Herein, we find that the photocatalytic CO2RR efficiency at the abundant gas‐liquid interface provided by microdroplets is two orders of magnitude higher than that of the corresponding bulk phase r...

Aerosol microdroplets as microreactors for many important atmospheric reactions are ubiquitous in the atmosphere. pH largely regulates the chemical processes within them; however, how pH and chemical species spatially distribute within an atmospheric microdroplet is still under intense debate. The challenge is to measure pH distribution within a ti...

Atmospheric deposition is an important source for the P biological cycle, especially for P‐limited ecosystems. In the present study, 48 hr size‐segregated aerosol samples were collected at an urban site in Shanghai for one year from May 2019 to June 2020. Total phosphorus (TP) presented a bimodal distribution in four seasons, which was mainly contr...

Solar‐driven CO 2 reduction reaction (CO 2 RR) is largely constrained by the sluggish mass transfer and fast combination of photogenerated charge carriers. Herein, we find that the photocatalytic CO 2 RR efficiency at the abundant gas‐liquid interface provided by microdroplets is two orders of magnitude higher than that of the corresponding bulk ph...

The ever-increasing NO emission has caused severe environmental issues and adverse effects on human health. Electrocatalytic reduction is regarded as a win-win technology for NO treatment with value-added NH3 generation, but the process is mainly relied on the metal-containing electrocatalysts. Here, we developed metal-free g-C3N4 nanosheets (depos...

Volatile organic compounds (VOCs) have important impacts on air quality, atmospheric chemistry and human health. In order to identify the spatiotemporal variations, sources and ozone (O3) and secondary organic aerosol (SOA) formation potentials of the atmospheric VOCs, a concurrent multi-site observation campaign was performed at the supersites of...

Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Here, we generated dust aerosols from soils to determine if there is particle size-dependent selectivity of heavy metals in the dust generation. Mn, Cd, Pb and other h...

Against the background of the current healthcare and climate emergencies, surface enhanced Raman scattering (SERS) is becoming a highly topical technique for identifying and fingerprinting molecules, e.g. within viruses, bacteria, drugs, and atmospheric aerosols. Crucial for SERS is the need for substrates with strong and reproducible enhancements...

The oxidative dissolution of As from arsenopyrite, one important arsenic mineral in reducing conditions, poses an environmental hazard to natural aquatic systems. The dissolution of arsenopyrite occurs slowly due to the surface precipitates of iron oxides in circumneutral oxic environments. However, the presence of natural ligands and coexisting me...

Fe(III)-oxalate complexes are ubiquitous in atmospheric environments, which can release reactive oxygen species (ROS) such as H2O2, O•2-, and OH• under light irradiation. Although Fe(III)-oxalate photochemistry has been investigated extensively, the understanding of its involvement in authentic atmospheric environments such as aerosol droplets is f...

Solar-driven H2O2 production is a promising approach for addressing both the energy and environmental crises. However, H2O2 photosynthesis is still restricted by the insufficient electron-hole separation efficiency (ηsep) and sluggish...

Nanoplastics (<1000 nm) have been evidenced to be universal in a variety of environmental media. They pose a potential cytotoxicity and health risk due to their tiny size, which allows them to easily penetrate biological barriers and enter cells. Here, we briefly review the various prevalent analytical techniques or tools for identifying nanoplasti...

People of all ages consume salt every day, but is it really just salt? Plastic nanoparticles (nanoplastics) polluting the oceans and the atmosphere are posing an increasing environmental threat and have begun to contaminate everyday salt in consumer goods. Herein, we developed a combined Surface Enhanced Raman Scattering (SERS) and Stimulated Raman...

Photochemical synthesis and photocatalysis in droplet microreactors represent promising approaches to relieve the global energy and environmental crises. Here, we describe a protocol for studying microdroplet photoreaction at an individual droplet level based on in situ micro-Raman spectroscopy. We provide details of superhydrophobic substrate prep...

Research on the microplastics (MPs) is developing towards smaller size, but corresponding methods for the rapid and accurate detection of microplastics, especially nanoplastics still present challenge. In this work, a novel surface and volume enhanced Raman spectroscopy substrate was developed for the rapid detection of microplastic particles below...

Flow velocity, potentially linked to dry deposition velocity and wind speed parameters, show non-marginal significance in the heterogeneous oxidation of SO2 on α-Fe2O3 particles. Our uptake measurement results produce lab-based evidence that an increase in flow velocity can potentially strengthen SO2 uptake capability over α-Fe2O3 by nearly one ord...

The importance of dust heterogeneous oxidation in the removal of atmospheric SO2 and formation of sulfate aerosols is not adequately understood. In this study, the Fe-, Ti-, and Al-bearing components, Na+, Cl-, K+, and Ca2+ of the dust surface, were discovered to be closely associated with the heterogeneous formation of sulfate. Regression models w...

Despite of the extensive research in semiconductor photocatalysis with respect to material and device innovations, much of the fundamental aquatic chemistry of those new materials that governs their environmental hazard and implications remains poorly understood. BiVO4 has long been recognized as a promising visible-light-responsive photocatalyst....

Emerging antibiotic resistant bacteria constitute one of the biggest threats to public health. Surface-enhanced Raman scattering (SERS) is highly promising for detecting such bacteria and for antibiotic susceptibility testing (AST). SERS is fast, non-destructive (can probe living cells) and it is technologically flexible (readily integrated with ro...

Solar‐driven CO 2 reduction reaction (CO 2 RR) is largely constrained by the sluggish mass transfer and fast combination of photogenerated charge carriers. Herein, we find that the photocatalysis CO 2 RR efficiency at the abundant gas-liquid interface provided by microdroplets is two orders of magnitude higher than that of the corresponding bulk ph...

Carbon dioxide is considered an inert gas that rarely participates in atmospheric chemical reactions. Nonetheless, we show here that CO2 is involved in some important photo-oxidation reactions in the atmosphere through the formation of carbonate radicals (CO3⚫-). This potentially active intermediate CO3⚫- is routinely overlooked in atmospheric chem...

Cooking is an important source of indoor emissions, and exposure to cooking emissions can instigate adverse health effects. Oxidative potential (OP) is a good indicator for assessing health risk, but studies detecting the OP of cooking emissions are rare. In this paper, size-segregated samples were collected at four sites in the canteen to study th...

Metal–organic frameworks (MOFs) are promising platforms for heterogeneous tethering of molecular CO2 reduction electrocatalysts. Yet, to further understand electrocatalytic MOF systems, one also needs to consider their capability to fine‐tune the immediate chemical environment of the active site, and thus affect its overall catalytic operation. Her...

Metal‐Organic Frameworks (MOFs) are promising platforms for heterogeneous tethering of molecular CO2 reduction electrocatalysts. Yet, to further understand electrocatalytic MOF systems, one also needs to consider their capability to fine‐tune the immediate chemical environment of the active site, and thus affect its overall catalytic operation. her...

The spatiotemporal concentration variations, sources, and secondary transformation potential of volatile organic compounds (VOCs) were analyzed at three sampling sites, including the rural (DSL), urban (PD) and industrial (JS) sites, in December 2019, in Shanghai, China. The VOC concentrations in the DSL, PD and JS sites were 13.32 ± 3.33 ppb, 24.7...

Photochemistry and photocatalysis are promising approaches to derive solar energy for solving the global energy and environment crisis. However, some practical aspects remain daunting, mainly due to the slow reaction kinetics, especially for multiphase reactions involving gaseous reactants. Here, we report that the oxidation of methyl orange, golde...

Volatile organic compounds (VOCs) have important impacts on air quality, climate, and human health. In order to identify the characteristics, sources and secondary formation potentials of the atmospheric VOCs varying with land use types, a concurrent multi-site observation campaign was performed at the supersites of Shanghai, East China, in the fir...

The importance of dust heterogeneous chemistry in the removal of atmospheric SO2 and formation of sulfate aerosols is not adequately understood. In this study, the Fe, Ti, Al-bearing components, Na+, Cl-, K+, and Ca2+ of the dust surface were discovered to be closely associated with the heterogeneous formation of sulfate. Regression models were the...

The world is facing a severe issue regarding microplastics (MPs) pollution, which is ascribed to its small micron size, low capture, and difficulties in removing it from the environment. The MPs' pollution control and removal policies throughout the world were a pioneering subject of plastics waste, but also a crucial problem that needs to be addre...

Nanotechnology has the potential to boost agricultural production by enabling nanosensors with electrical, optical, mechanical, and wireless properties for improving the agricultural practices. Reducing crop yield, pathogen attack, and environmental stresses are the major challenges faced worldwide. New and advance technologies are required for eff...

Iron oxyhydroxide (FeOOH) is one of the most abundant atmospheric iron oxides. Considering their diverse emission features and reaction processes, airborne FeOOH minerals present distinct crystal structures and coating compositions....

An efficient degradation method for microplastics treatment is urgently needed. In this review, a comprehensive overview of current methods of microplastics degradation, including biological, photo, chemical, and mechanical degradation, are summarized and discussed.

Correction for ‘Surface-enhanced Raman spectroscopy for bioanalysis and diagnosis’ by Muhammad Ali Tahir et al. , Nanoscale , 2021, 13 , 11593–11634, DOI: 10.1039/D1NR00708D.

We analysed the biogenic volatile organic compound (BVOC) emissions from rapeseed leaf litter and their potential to create secondary organic aerosols (SOAs) under three different conditions, i.e., (i) in the presence of UV light irradiation, (ii) in the presence of ozone, and (iii) with both ozone and UV light. These experiments were performed in...

Carbon dioxide is considered an inert gas that rarely participates in atmospheric chemical reactions. However, we show here that CO2 is involved in some important photo-oxidation reactions in the atmosphere through the formation of carbonate radicals (CO3∙-). This potentially active intermediate CO3∙- is routinely overlooked in atmospheric chemistr...

In recent years, bioanalytical surface-enhanced Raman spectroscopy (SERS) has blossomed into a fast-growing research area. Owing to its high sensitivity and outstanding multiplexing ability, SERS is an effective analytical technique that has excellent potential in bioanalysis and diagnosis, as demonstrated by its increasing applications in vivo. SE...

The advancement in industries and modern technology has been escorted by an expansion in the utilization of chemicals to obtain plastic-based products. Increased plastic production and disposal have greatly affected the environment and living organisms globally. Macro and micro-plastics have a persistent nature, and their natural degradation takes...

Herein, electronic structure of carbon nitride is reconstructed and tailored by simply calcining the sodium borohydride and CN nanosheets (CNS) in a nitrogen atmosphere, which could promote the in-plane separation and transport of charge carriers. Accordingly, structural reconstruction of CNS manifests outstanding CO2 reduction performance (55.3 μm...

Microdroplets present unique physiochemical properties, which can influence chemical reactions and atmospheric aerosol processes. The microdroplets’ pH is one of the most important factors that dictate chemical processes, such as heterogeneous and condensed reactions. However, currently, there is no well-established method for directly measuring th...

Photocatalysis has been regarded as a sustainable strategy for wastewaters remediation, and sulfite addition could significantly accelerate the photocatalytic performances. However, the related mechanisms are still not well understood. Here, we for the first time found that plasmonic Bi and oxygen vacancies were in-operando generated on BiOX (X = C...

Among the possible products of CO2 electrochemical reduction, CO plays a unique and vital role, which can be an ideal feedstock for further reduction to C2+ products, and also the important component of syngas that can be used as feedstock for value-added chemicals and fuels. However, it is still a challenge to tune the CO selectivity on Cu electro...

Photochemical reaction of NO2 on semiconductor is of scientific significance in both photocatalytic NOx removal and nitrogenous aerosol formation. A fundamental understanding of the reaction mechanism and how irradiation intensity influences the product distribution and reaction kinetics remains uncertain. By means of DRIFTS (diffuse reflection inf...

Monolayer-ordered gold nanoring arrays were prepared by ion-sputtering method and used as surface enhanced Raman spectroscopy (SERS) substrates to test the individual atmospheric aerosols particle. Compared to other methods used for testing atmospheric aerosols particles, the collection and subsequent detection in our work is performed directly on...

Water soluble low-molecular-weight dicarboxylic acids (DCAs) and corresponding salts are ubiquitous in the atmosphere. They could efficiently form chelate with iron in atmospheric particles, which could be photoexcited to generate a series of strong oxidants and have profound impacts on atmospheric chemistry. However, the influences of iron-DCAs co...

Heavy loadings of sulfate aerosol trigger haze formation and pose great damage to human health in Taiwan Island. Nevertheless, high-resolution spatiotemporal variation of ambient sulfate across Taiwan Island still remained unknown because of the scarce monitoring sites. Thus, we developed a novel ensemble model named extreme gradient boosting coupl...

In this study, direct conversion of rice straw to ethyl lactate (EL) was evaluated in acidic conditions with ethanol as reaction medium. The devised Lewis acid catalyst system (SnCl2/SnCl4) and, Lewis/Brønsted acid catalyst system (SnCl2/ZSM-5) played vital role in the selective production of EL. The yield of EL was optimized up to 21.8% with SnCl2...

Water-soluble organic carbon (WSOC), which is closely related to biogenic emissions, is of great importance in the atmosphere for its ubiquitous existence and rich abundance. Levoglucosan, a typical WSOC, is usually considered to be stable and thus used as a tracer of biomass burning. However, we found that levoglucosan can be photo-oxidized on min...

Micro- and nanoplastics are considered one of the top pollutants that threaten the environment, aquatic life, and mammalian (including human) health. Unfortunately, the development of uncomplicated but reliable analytical methods that are sensitive to individual microplastic particles, with sizes smaller than 1 μm, remains incomplete. Here, we demo...

Dissolved Mn(III) species have been recognized as a significant form of Mn in redox transition environments, but a holistic understanding of their geochemical properties still lacks the characterization of their reactivity as reductants. Through using PbO2 as a surrogate oxidant and pyrophosphate (PP) as a model ligand, we evaluated the thermodynam...

Recent research has shown that the complexation of metals-organics plays an important role in atmospheric particulate matter, whose health effects should be taken into account. This work investigates the interactions between catechols (CAs), i.e., 4-nitrocatechol (4NC) and 4-methylcatechol (4MC), and transition metals (i.e., Fe) in the aqueous phas...

The heterogeneous reaction of SO2 on manganese oxides is poorly understood. By means of in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS), this study investigated the reaction kinetics and product fractions on four types of manganese oxides. Due to the positive and negative moisture impacts, 68% RH (relative humidity) bec...

Recently, the environmental impacts of microplastics have received extensive attention due to their accumulation in the environment. However, developing efficient technology for the control and purification of microplastics is still a big challenge. Herein, we investigated the photocatalytic degradation of typical microplastics such as polystyrene...

The electrocatalytic transformation of carbon dioxide to higher value hydrocarbons offers opportunities for large scale, long term renewable energy storage and lessen carbon emissions. The fabrication of an efficient electrocatalyst with high selectivity for multicarbon (C2) products remains a topic of continuous interest. Here we report, highly de...

The rapid sulfate formation is a crucial factor determining the explosive growth of fine particles and the frequent occurrence of severe haze events in China. Recent field observations also show that brown carbon is one of the most critical components in aerosol particles sampled during haze episodes. To this day, there is limited knowledge that ac...