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The levels of air pollution in Macao often exceeded the levels recommended by WHO. In order for the population to take precautionary measures and avoid further health risks under high pollutant exposure, it is important to develop a reliable air quality forecast. Statistical models based on linear multiple regression (MR) and classification and regression trees (CART) analysis were developed successfully, for Macao, to predict the next day concentrations of NO2, PM10, PM2.5, and O3. All the developed models were statistically significantly valid with a 95% confidence level with high coefficients of determination (from 0.78 to 0.93) for all pollutants. The models utilized meteorological and air quality variables based on 5 years of historical data, from 2013 to 2017. Data from 2013 to 2016 were used to develop the statistical models and data from 2017 was used for validation purposes. A wide range of meteorological and air quality variables was identified, and only some were selected as significant independent variables. Meteorological variables were selected from an extensive list of variables, including geopotential height, relative humidity, atmospheric stability, and air temperature at different vertical levels. Air quality variables translate the resilience of the recent past concentrations of each pollutant and usually are maximum and/or the average of latest 24-h levels. The models were applied in forecasting the next day average daily concentrations for NO2 and PM and maximum hourly O3 levels for five air quality monitoring stations. The results are expected to be an operational air quality forecast for Macao.

Statistical methods such as multiple linear regression (MLR) and classification and regression tree (CART) analysis were used to build prediction models for the levels of pollutant concentrations in Macao using meteorological and air quality historical data to three periods: (i) from 2013 to 2016, (ii) from 2015 to 2018, and (iii) from 2013 to 2018. The variables retained by the models were identical for nitrogen dioxide (NO2), particulate matter (PM10), PM2.5, but not for ozone (O3) Air pollution data from 2019 was used for validation purposes. The model for the 2013 to 2018 period was the one that performed best in prediction of the next-day concentrations levels in 2019, with high coefficient of determination (R2), between predicted and observed daily average concentrations (between 0.78 and 0.89 for all pollutants), and low root mean square error (RMSE), mean absolute error (MAE), and biases (BIAS). To understand if the prediction model was robust to extreme variations in pollutants concentration, a test was performed under the circumstances of a high pollution episode for PM2.5 and O3 during 2019, and the low pollution episode during the period of implementation of the preventive measures for COVID-19 pandemic. Regarding the high pollution episode, the period of the Chinese National Holiday of 2019 was selected, in which high concentration levels were identified for PM2.5 and O3, with peaks of daily concentration exceeding 55 μg/m3 and 400 μg/m3, respectively. The 2013 to 2018 model successfully predicted this high pollution episode with high coefficients of determination (of 0.92 for PM2.5 and 0.82 for O3). The low pollution episode for PM2.5 and O3 was identified during the 2020 COVID-19 pandemic period, with a low record of daily concentration for PM2.5 levels at 2 μg/m3 and O3 levels at 50 μg/m3, respectively. The 2013 to 2018 model successfully predicted the low pollution episode for PM2.5 and O3 with a high coefficient of determination (0.86 and 0.84, respectively). Overall, the results demonstrate that the statistical forecast model is robust and able to correctly reproduce extreme air pollution events of both high and low concentration levels.

Air pollution is a major concern issue on Macao since the concentration levels of several of the most common pollutants are frequently above the internationally recommended values. The low air quality episodes impacts on human health paired with highly populated urban areas are important motivations to develop forecast methodologies in order to anticipate pollution episodes, allowing establishing warnings to the local community to take precautionary measures and avoid outdoor activities during this period. Using statistical methods (multiple linear regression (MLR) and classification and regression tree (CART) analysis) we were able to develop forecasting models for the main pollutants (NO2, PM2.5, and O3) enabling us to know the next day concentrations with a good skill, translated by high coefficients of determination (0.82–0.90) on a 95% confidence level. The model development was based on six years of historical data, 2013 to 2018, consisting of surface and upper-air meteorological observations and surface air quality observations. The year of 2019 was used for model validation. From an initially large group of meteorological and air quality variables only a few were identified as significant dependent variables in the model. The selected meteorological variables included geopotential height, relative humidity and air temperature at different altitude levels and atmospheric stability characterization parameters. The air quality predictors used included recent past hourly levels of mean concentrations for NO2 and PM2.5 and maximum concentrations for O3. The application of the obtained models provides the expected daily mean concentrations for NO2 and PM2.5 and maximum hourly concentrations O3 for the next day in Taipa Ambient air quality monitoring stations. The described methodology is now operational, in Macao, since 2020.

Despite the levels of air pollution in Macao continuing to improve over recent years, there are still days with high-pollution episodes that cause great health concerns to the local community. Therefore, it is very important to accurately forecast air quality in Macao. Machine learning methods such as random forest (RF), gradient boosting (GB), support vector regression (SVR), and multiple linear regression (MLR) were applied to predict the levels of particulate matter (PM10 and PM2.5) concentrations in Macao. The forecast models were built and trained using the meteorological and air quality data from 2013 to 2018, and the air quality data from 2019 to 2021 were used for validation. Our results show that there is no significant difference between the performance of the four methods in predicting the air quality data for 2019 (before the COVID-19 pandemic) and 2021 (the new normal period). However, RF performed significantly better than the other methods for 2020 (amid the pandemic) with a higher coefficient of determination (R2) and lower RMSE, MAE, and BIAS. The reduced performance of the statistical MLR and other ML models was presumably due to the unprecedented low levels of PM10 and PM2.5 concentrations in 2020. Therefore, this study suggests that RF is the most reliable prediction method for pollutant concentrations, especially in the event of drastic air quality changes due to unexpected circumstances, such as a lockdown caused by a widespread infectious disease.

Hydrothermal activity on mid-ocean ridges is an important mechanism for the delivery of Zn from the mantle to the surface environment. Zinc isotopic fractionation during hydrothermal activity is mainly controlled by the precipitation of Zn-bearing sulfide minerals, in which isotopically light Zn is preferentially retained in solid phases rather than in solution during mineral precipitation. Thus, seafloor hydrothermal activity is expected to supply isotopically heavy Zn to the ocean. Here, we studied sulfide-rich samples from the Duanqiao-1 hydrothermal field, located on the Southwest Indian Ridge. We report that, at the hand-specimen scale, late-stage conduit sulfide material has lower δ66Zn values (−0.05 ± 0.15 ‰; n = 19) than early-stage material (+0.13 ± 0.15 ‰; n = 10). These lower values correlate with enrichments in Pb, As, Cd, and Ag, and elevated δ34S values. We attribute the low δ66Zn values to the remobilization of earlier sub-seafloor Zn-rich mineralization. Based on endmember mass balance calculations, and an assumption of a fractionation factor (αZnS-Sol.) of about 0.9997 between sphalerite and its parent solution, the remobilized Zn was found consist of about 1/3 to 2/3 of the total Zn in the fluid that formed the conduit samples. Our study suggests that late-stage subsurface hydrothermal remobilization may release isotopically-light Zn to the ocean, and that this process may be common along mid-ocean ridges, thus increasing the size of the previously identified isotopically light Zn sink in the ocean.

The on-board identification of ore minerals during a cruise is often postponed until long after the cruise is over. During the M127 cruise, 21 cores with deep-seafloor sediments were recovered in the Trans-Atlantic Geotraverse (TAG) field along the Mid Atlantic Ridge (MAR). Sediments were analyzed on-board for physicochemical properties such as lightness (L*), pH and Eh. Selected samples were studied for mineral composition by X-ray powder diffraction (XRD). Based on XRD data, sediment samples were separated into high-, low- and non-carbonated. Removal of carbonates is a common technique in mineralogical studies in which HCl is used as the extraction agent. In the present study, sequential extraction was performed with sodium acetate buffer (pH 5.0) to remove carbonates. The ratio between the highest calcite XRD reflection in the original samples (Iorig) vs its XRD-reflection in samples after their treatment with the buffer (Itreat) was used as a quantitative parameter of calcite removal, as well as to identify minor minerals in carbonated samples (when Iorig/Itreat > 24). It was found that the lightness parameter (L*) showed a positive correlation with calcite XRD reflection in selected TAG samples, and this could be applied to the preliminary on-board determination of extraction steps with acetate buffer (pH 5.0) in carbonated sediment samples. The most abundant minerals detected in carbonated samples were quartz and Al- and Fe-rich clays. Other silicates were also detected (e.g., calcic plagioclase, montmorillonite, nontronite). In non-carbonated samples, Fe oxides and hydroxides (goethite and hematite, respectively) were detected. Pyrite was the dominant hydrothermal mineral and Cu sulfides (chalcopyrite, covellite) and hydrothermal Mn oxides (birnessite and todorokite) were mineral phases identified in few samples, whereas paratacamite was detected in the top 20 cm of the core. The present study demonstrates that portable XRD analysis makes it possible to characterize mineralogy at cored sites, in particular in both low- and high-carbonated samples, before the end of most cruises, thus enabling the quick modification of exploration strategies in light of new information as it becomes available in near-real time.

The geochemistry and mineralogy of sediments provide relevant information for the understanding of the origin and metallogenic mechanism of ferromanganese nodules and crusts. At present, there are still few studies on the sediment origin of the Clarion–Clipperton Zone (CCZ) of the east Pacific, particularly on the systematic origin of sediments with a longer history/length. Here, bulk sediment geochemistry and clay mineral compositions were analyzed on a 5.7 m gravity core (GC04) obtained at the CCZ, an area rich in polymetallic nodules. The results indicate that the average total content of rare earth elements (REE), including yttrium (REY), in sediments is 454.7 ppm and the REEs distribution patterns normalized by the North American Shale Composite of samples are highly consistent, with all showing negative Ce anomalies and more obvious enrichment in heavy REE (HREE) than that of light REE (LREE). Montmorillonite/illite ratio, discriminant functions and smear slide identification indicate multiple origins for the material, and are strongly influenced by contributions from marine biomass, while terrestrial materials, seamount basalts and their alteration products and authigenic source also make certain contributions. The REY characteristics of the sediments in the study area are different from those of marginal oceanic and back-arc basins, and more similar to pelagic deep-sea sediments. Based on LREE/HREE-1/δCe and LREE/HREE-Y/Ho diagrams, we conclude that samples from the study area had pelagic sedimentary properties which suffered from a strong “seawater effect”.

Macao ( 30 Km2) is a territory characterized by small granitic intrusions, located along the coastal region of Southeast China (Cathaysia Block). Granitoids occur as different facies, including microgranite dykes, with distinct textural, mineralogical and geochemical features, for which a middle-upper Jurassic age ( 164 Ma) has been proposed. New data suggest that these granitoids are mostly high-K calc-alkaline metaluminous (A/CNK = 0.8 - 1.1) biotite granites, consistent with total absence of primary muscovite. They show variable amounts of SiO2 (67-77%), reflecting different degrees of magmatic evolution. There is also variability in terms of trace elements, particularly Rare Earth Elements (REEs), evidenced by decreasing (La/Sm)N, (Gd/Lu)N, (Ce/Yb)N and (Eu/Eu*)N towards the more evolved samples, which can be partly attributed to fractional crystallization processes. Most of the granitoids are characterized by (La/Yb)N = 3 - 10.8, showing negative Ba, Nb, Sr, Zr, P, Ti and Eu anomalies. On the other hand, microgranite dykes, along with a few more evolved granites, show an opposite tendency, being usually enriched in HREEs relatively to LREEs with (La/Yb)N = 0.4 - 1.1. Our data suggests intermediate genetic affinities between I-type and A-type granites. Although these granitoids are mostly metaluminous (characteristic of I-types), Ga/Al ratios, usually used to identify A-types, are close to the accepted boundary between A-type and other granite types. The affinities with A-type granites are more marked for the more evolved facies, which depict higher values of FeOt/MgO (14 - 60) and K2O/MgO (60 - 250). Their trace element characteristics are also transitional between WPG (Within-plate granites) and Syn-COLG (Collision Granites). We interpret those transitional characteristics (A/I and WPG/Syn-COLG) of Macao granitoids as reflecting an origin by melting of infracrustal sources over a period of high heat transfer from mantle to crust during an extensional tectonic setting probably contemporaneous with the subduction of the paleo-Pacific plate beneath the Eurasia, whose paleo-suture is thought to be located in the east flank of the Central Range, Taiwan.

The territory of Macao is composed of several granitic intrusions belonging to one of the biggest granite provinces in the world, the Southeast China Magmatic Belt (SCMB), located in the southeast (SE) area of the Cathaysia Block. The SCMB is known by the occurrence of large volumes of Mesozoic magmatic rocks (over 90% are granitic rocks and equivalent volcanic rocks with minor basalts), occupying a total outcrop area of nearly 200.000 km2. The geology of Macao (~30 Km2) is dominated by granitic rocks displaying a wide range of textural, mineralogical and chemical features, making it an ideal region to study these rocks and the petrogenetic processes responsible for their diversity. This study employed a wide range of research methodologies, namely field studies, petrography, zircon geochronology, mineral chemistry, whole-rock elemental and isotopic geochemistry to determine the nature of the source, the petrogenetic processes and the tectonic regimes of the Mesozoic magmatism in this region. Thus, the data collected along this study aims to provide new knowledge on the tectono-magmatic evolution of Macao, in particular, and of SE China, in general. The results obtained from the high-precision U–Pb zircon geochronology, acquired through isotope dilution thermal ionization mass spectrometry (ID-TIMS) and in-situ laser ablation multi-collector inductively coupled mass spectrometry (LA-MC-ICPMS), revealed different ages for Macao granites. Despite its relatively small area, the determined ages tightly constrain the Macao granitic magmatism to two periods, ranging from 164.5 ± 0.6 to 162.9 ± 0.7 Ma (MGI – Macao Group I granites) and 156.6 ± 0.2 to 155.5 ± 0.8 Ma (MGII – Macao Group II granites). In addition, younger dacitic rocks were dated at 150.6 ± 0.6 Ma and <120 Ma. The existence of two proximal but distinct granitic pulses, spanning for a time of about 9 Ma and separated by ca. 6 Ma, in the Macao granitic suite suggests that it was incrementally assembled. This hypothesis is also extendable to the neighbouring Hong Kong region, where the magmatic activity occurred in four major pulses spanning for about 24 Ma. However, the MGII granites indicate the occurrence, on the Pearl River Delta region, of a magmatic pulse between those defined in Hong Kong at the origin of Lamma Suite (165–160 Ma) and the Kwai Chung Suite (148–146 Ma). In addition, Rare Element Earth (REE) ratios suggest that this pulse may only occur in Macao area, while MGI granites show evolving trends of REE ratios similar to those of Jurassic granites outcropping in vast areas of the Cathaysia Block (SE China). Inheritance patterns in the zircon U–Pb data indicate the presence of a population of antecrysts (165–180 Ma) crystallized from earlier magmatic pulses and a population of inherited zircons, from Precambrian to Phanerozoic sources, incorporated into the magmas during melting and/or ascent/emplacement at crustal levels. The oldest inherited ages (2.4 Ga and possibly 2.9 Ga) suggest contribution of Proterozoic and possibly of late Archaean crustal sources for the Macao magmatism. The granitic rocks of Macao are mainly high-K calc-alkaline metaluminous to weakly peraluminous I-type granites with variable degrees of fractionation. Fractional crystallization played an important role in the evolution of these granites, though the fractionation paths differ for the highly fractionated facies of both groups mainly due to distinct accessory fractionating phases. Such difference is evident by distinct REE evolution trends: while MGI magmas seem to have evolved by gradual enrichment in heavy REE relatively to light REE, originating progressively flatter REE patterns, magmas from MGII are marked by depletion of middle REE, leading to progressively concave upward REE patterns. However, while most of the geochemical variation of the MGII granites can be explained by fractional crystallization, the same is not true for MGI granites. The MGI highly fractionated granites show evidence for the REE tetrad effect and are characterized by non-CHArge-and-RAdius-Controlled (non-CHARAC) behaviour of trace elements, suggesting late-stage melt/fluid interactions involving F-rich fluids. The stage of evolution represented by the MGI highly fractionated granites corresponds to the onset of fluid/melt interaction in a highly evolved granitic system, which may have led to enhanced hydrothermal activity in more evolved stages, as those represented in neighbouring areas in SE China. Significant differences in isotopic composition were also observed, with the MGII being characterized by a much narrow range of initial 87Sr/86Sr ratios and εNd(t) and εHf(t) values than MGI. Based on these differences, the MGII granites are considered to be part of a comagmatic suite that has evolved in closed system, contrasting with what can be inferred for MGI. The increase in initial 87Sr/86Sr ratios with degree of evolution, the presence of metasedimentary enclaves and the high percentage of inherited zircon with Paleozoic ages in MGI, suggest the occurrence of an assimilation fractionation crystallization (AFC) process. The AFC processes were a major cause for the I-S transitional characteristics of the MGI highly fractionated granites and possibly of the other similar Jurassic biotite granites in SE China. The observed decoupling of Sr, Nd and Hf isotope systems might have resulted from magma mixing between the granitic and more mafic magmas, which caused the homogenization of Sr isotope ratios but not of the Nd and Hf ones. Such process is also supported by the occurrence of Microgranular Mafic Enclaves (MME) hosted by the granites. Isotope and major element compositions together with model ages strongly suggest that Macao granitic magmas were generated by partial melting of infracrustal medium-to-high K basaltic Paleo-Proterozoic to Mesoproterozoic protoliths heated by, and mixed to some degree with mantle-derived magmas. The temporal and spatial association of Macao and SE China Jurassic I-type granites with basaltic/gabbroic rocks, syenites and A-type granites, displaying typical intraplate chemical features, indicates an extensional regime rather than an active margin for the origin of these rocks. It also points to an important role of mantle-derived magmas in the production of SE China Jurassic granites. Adiabatic decompression melting of the asthenospheric mantle produced mafic magmas, which underplated at the base of the crust (Moho), subsequently triggering partial melting of the lower crust to generate the granitic magmas. The Jurassic Macao granites are interpreted as being produced in an intraplate extensional setting related to the break-off and foundering of a previously flat-slab (Paleo-Pacific plate) beneath the Eurasian plate. The boundary between east and west Cathaysia blocks is roughly along the Zhenghe-Dapu Fault (ZDF), which intersects the SE China coast near Hong Kong and is thought to have played a major role for the Mesozoic magmatic activity in this region. The stronger isotopic affinities of Macao granites with the other granitic rocks and lower crustal xenoliths from the western Cathaysia Block suggest that the ZDF is likely to pass south of Macao, a fact that has not been mentioned before. In addition to the Early Yanshanian (Jurassic) granitic magmatism in Macao, the younger ages obtained for the dacite dykes indicate that the territory was also affected, to a lesser degree, by Late Yanshanian (Cretaceous) magmatism. The transition from granitic to dacitic magmatism most likely corresponds to a change in the regional tectonic regime, which induced a significant change in the magma genesis processes. In contrast with the intraplate features of Macao and SE China Jurassic granites and coeval mafic rocks, the geochemical features of the Macao dacite dykes (e.g. high LILE/HFSE ratios and negative anomalies of Nb, Ta and Ti) are identical to those characterizing arc-like subduction-related magmas. These dacites are most likely evolved products of arc-like magmatism and may testify the reestablishment of a normal subduction system in this area of SE China.

A 1:12,000 geological map of the Macao Special Administrative Region has been produced through detailed field work supported by petrographic, mineralogical, geochronological and geochemical data obtained in previous studies. This map aims to represent a reliable tool to understand the geological evolution of the region and for management of the territory. The geology of Macao is dominated by two groups of Jurassic granitic rocks belonging to an intrusive suite located along the coast of Southeast China: Macao Group I (MGI: 164.5 ± 0.6 to 162.9 ± 0.7 Ma) and Macao Group II (MGII: 156.6 ± 0.2 to 155.5 ± 0.8 Ma), including the associated microgranite, aplite and pegmatite dikes and quartz veins. Remnants of the metasedimentary wall-rock are present as Devonian xenoliths enclosed within the granites. Younger Jurassic to Cretaceous andesite to dacite dikes (150.6 ± 0.6 to <120 Ma) intrude the granitic rocks. Additionally, Quaternary sedimentary deposits cover the older lithologies.

Abstract Much controversy has occurred in the past few decades regarding the nature of the sources, the petrogenetic processes, and the tectonic regime(s) of the Jurassic magmatism within the Southeast China magmatic belt. This study aims to contribute to the discussion with mineral chemistry, and whole-rock element and Sr-Nd-Hf-Pb isotopic geochemical data from granitic rocks and microgranular mafic enclaves from Macao, where two discrete groups of I-type biotite granites have been identified (referred to as Macao Group I [MGI] and Macao Group II [MGII]). It is proposed that the granitic magmas were generated by partial melting of infracrustal medium- to high-K, basaltic Paleoproterozoic to Mesoproterozoic protoliths (Nd depleted mantle model age [TDM2] = 1.7–1.6 Ga and Hf TDM2 = 1.8–1.6 Ga), triggered by underplating of hot mantle-derived magmas in an extensional setting related to the foundering of a previously flat slab (paleo–Pacific plate) beneath the SE China continent. The main differences between the two groups of Macao granites are attributed to assimilation and fractional crystallization processes, during which upper-crustal Paleozoic metasediments were variably assimilated by MGI magmas. This is evidenced by an increase in initial 87Sr/86Sr ratios with degree of evolution, presence of metasedimentary enclaves, and high percentage of zircon xenocrysts with Paleozoic ages. In addition, other processes like late-stage fluid/melt interaction and magma mixing also left some imprints on granite compositions (rare earth element tetrad effect plus non–charge-and-radius-controlled behavior of trace elements and decoupling between different isotope systems, respectively). The distribution of isotopically distinct granites in SE China reflects the nature of the two Cathaysia crustal blocks juxtaposed along the Zhenghe-Dapu fault.

The widespread W-(Mo)-Sn-Nb-Ta polymetallic mineralization in Southeast (SE) China is genetically associated with Mesozoic highly fractionated granitic rocks. Such rocks have enigmatic mineralogical and geochemical features, making its petrogenesis an intensely debated topic. To better understand the underlying magma evolution processes, petrography, garnet chemistry and whole-rock major and trace element data are reported for Jurassic highly fractionated granitic rocks and associated microgranite and aplitepegmatite dikes from Macao and compared with coeval similar granitic rocks from nearby areas in SE China. Despite the fact that the most evolved rocks in Macao are garnet-bearing aplite-pegmatite dikes, the existence of coeval two-mica and garnet-bearing biotite and muscovite granites displaying more evolved compositions (e.g, lower Zr/Hf ratios) indicates that the differentiation sequence reached higher degrees of fractionation at a regional scale. Although crystal fractionation played an important role, late-stage fluid/melt interactions, involving F-rich fluids, imparted specific geochemical characteristics to Macao and SE China highly fractionated granitic rocks such as the non-CHARAC (CHArge-and-RAdius-Controlled) behavior of trace elements, leading, for example, to non-chondritic Zr/Hf ratios, Rare Earth Elements (REE) tetrad effects and Nb-Ta enrichment and fractionation. Such process contributed to the late-stage crystallization of accessory phases only found in these highly evolved facies. Among the latter, two populations of garnet were identified in MGI (Macao Group I) highly fractionated granitic rocks: small grossular-poor euhedral grains and large grossular-rich skeletal garnet grains with quartz inclusions. The first group was mainly formed through precipitation from highly evolved Mn-rich slightly peraluminous melts under low-pressure and relatively low temperature (∼700 °C) conditions. Assimilation of upper crust metasedimentary materials may have contributed as a source of Mn and Al to the formation of garnet. The second group has a metasomatic origin related to the interaction of magmatic fluids with previously crystallized mineral phases and, possibly, with assimilated metasedimentary enclaves or surrounding metasedimentary strata. The highly fractionated granitic rocks in Macao represent the first stage in the development of granite-related W-(Mo)-Sn-Nb-Ta mineralization associated with coeval more evolved lithotypes in SE China.