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Water Resource Research

Supporting Information for

Global anthropogenic phosphorus loads to fresh water, grey water footprint and water pollution level: A high-resolution global study

Mesfin M. Mekonnen1,2 and Arjen Y. Hoekstra1,3

1 Twente Water Centre, University of Twente, P.O. Box 217, 7500 AE Enschede, The Netherlands

2 Robert B. Daugherty Water for Food Global Institute at the University of Nebraska, 2021 Transformation Dr., Ste 3220, Lincoln, NE 68583, USA

3 Institute of Water Policy, Lee Kuan Yew School of Public Policy, National University of Singapore, 469A Bukit Timah Road, 259770, Singapore.

Corresponding author: Mesfin Mekonnen (mmekonnen2@unl.edu).

Contents of this file

Text S1 and S2 Figures S1 Tables S1 to S6

Introduction

The supporting information provides a detailed description of the method used and the data input in the current study (Text S1) as well as additional results (Text S2).

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Text S1: Method and data

Text S1.1 Diffuse sources of phosphorus

Diffuse P loads to fresh water from agriculture were estimated for 126 crops separately by accounting the P inputs to

the soil through mineral fertilizer (INfer), manure (INman) and irrigation (INirr), and P removal with crop harvest

(OUTharv) and crop residues (OUTres) at a spatial resolution of 5×5 arc-minute.

Inputs from mineral fertilizers (INfer)

The fertilizer application rate per crop per country was calculated using three sources of fertilizer data and the spatially

explicit data on crop distribution from Monfreda et al. [2008]. IFA et al. [2002] provide fertilizer application rates per

crop for 88 countries. FAO [2012b] and Heffer [2009] were used to complement data for crops and countries missing

from the IFA et al. [2002] data. Since the application rates provided in these data sources is for different years, these

were adjusted to fit FAO [2012a] country average nutrient fertilizer consumption per year for the period 2002-2009.

Inputs from animal manure (INman)

The manure input was calculated at grid cell level by multiplying livestock density by the animal-specific excretion

rates. The volume of manure actually applied on cropland was estimated by accounting for the collection rate and the

allocation of collected manure over croplands versus pasture. We considered manure inputs on croplands (including

managed grasslands), but did not further study manure inputs on grazing lands.

Total manure P production within the grazing, mixed and industrial animal production systems for the major livestock

categories (cattle, buffaloes, sheep, goats, pigs and poultry) was calculated by multiplying the spatially explicit global

livestock density (taken from FAO [2012c]) with animal-specific excretion rates and then adjusted for the fraction of

manure available for cropland and grassland application [Bouwman et al., 2009; Bouwman et al., 2013; Liu et al.,

2010].

The manure P production per production system per animal category per grid cell (Mexc, kg P/ha) was calculated as

follows:

𝑀"#$[𝑎, 𝑠] = 𝐷[𝑎, 𝑠] × 𝐸[𝑎, 𝑐, 𝑠] (1)

where D[a, s] is the density of animal category a for production system s (head/ha) and E[a,c, s] the nutrient excretion

rate of animal category a in country c and production system s (kg P/head).

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(a)

(b)

Figure S1. Simplified representation of the model: (a) to estimate the anthropogenic P loads from both diffuse and point sources, and the associated GWF and WPL, and (b) to estimate manure excretion and its distribution on crop and grass land.

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To calculate the manure (P) excretion rate per animal category per country we followed the approach of Liu et al.

[2010]. Sheldrick et al. [2003] provide data on animal manure excretion rates for cattle, pigs, sheep, goats, and poultry

relative to the animals slaughter weight. The manure excretion rate per animal category, production system and

country was calculated by combining Sheldrick et al. [2003] global average manure excretion rates with slaughter

weight of animals per production systems and per country:

𝐸[𝑎, 𝑐, 𝑠] = /0[1,$,2]/03456[1]

× 𝐸27"8[𝑎] (2)

where SW[a,c,s] is the slaughter weight of animal category a (kg/head) in country c and production system s, SWshel[a]

the global average slaughter weight of animal category a (kg/head) and E[a] the global average manure excretion by

animal category a (kg/y), both obtained from Sheldrick et al. [2003]. The slaughter weights (SW[a,c,s]) of the different

animal category per production systems per country was obtained from Mekonnen and Hoekstra [2010b].

We can distinguish three types of manure within each production system and country [Bouwman et al., 2009;

Bouwman et al., 2013]: (a) manure produced from animals housed in stables, (b) manure produced from livestock

grazing on pasture or rangeland, and (c) manure excreted for example in urban areas, forests and along roadsides and

manure used as fuel or for other purposes that are considered to fall outside the agricultural system:

𝑀"#$[𝑎, 𝑠] = 𝑀2:;

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estimate which crops get what amount of manure, we allocated the manure per crop inversely proportional to their

share of the mineral fertilizer application: crops that got small amount of mineral fertilizer got more manure and those

that got large amount of mineral fertilizer got smaller manure.

The manure allocation needs to be corrected in some grid cells where the manure application rate was unrealistic. In

this case we had to do modification of the manure distribution by redistributing the excess manure to other grid cells

and crops within a country: we first collect all the excess manure within a country then redistribute to other grid cells

proportional to the cultivated area. This was we try to avoid unrealistic P application rate. But please not that, this

correction was not necessary in the majority of places.

Inputs from irrigation water (INirr)

The nutrient input in irrigation water is calculated for irrigated cropland by multiplying the P content of irrigation

water (in kg P/m3) by the irrigation application rate (in m3/ha per year). We adopted the average P content of irrigation

water as provided by Lesschen et al. [2007]: 0.4 mg/l. The irrigation application rate at 5×5 arc-minute spatial

resolution for all crops under irrigation condition was obtained from Mekonnen and Hoekstra [2010a].

Outputs from harvested crop and grass (OUTharv)

The P withdrawal in the harvested crops is calculated by multiplying the crop production by the P content of the crops.

P loss through harvested crop (OUTharv, kg P/ha) is calculated by aggregating the nutrient withdrawal from each crop

harvested and adding the nutrient withdrawal due to grass consumption and harvest as follows:

𝑂𝑈𝑇71

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where CR[r] is the volume of crop residue r (tonne/ha), p[r] the P content of residue r (kg P/tonne of crop residue),

and γ[r] the removal factor of the crop residue r. The nutrient contents of the crop residues were taken mainly from

IPNI [2012] and FAO [2004] and for a few crops from Roy et al. [2006]. Missing values for nuts and spices were

filled by adopting the values of fruits and vegetables respectively from FAO [2004]. The volume of crop residue was

calculated by multiplying dry crop yield with a residue-to-product ration (RPR). The RPR values for a large number

of crops and crop groupings were obtained from Eisentraut [2010]. For spices, we took the RPR values of vegetables.

The crop residue removal factors in Ghana, Kenya and Mali for various crops were obtained from FAO [2004].

Removal factors for 18 crops or crop groups in India were derived from Ravindranath et al. [2005]. For other crops

which are not covered by Ravindranath et al. [2005], we used the average removal factor of the 18 crops. For the USA,

crop residue removal factors for maize and wheat for a large number of states were obtained from Graham et al. [2007]

and Nelson et al. [2002], respectively. Removal factors of maize and wheat in other states were taken as the average

removal factor in the states with data. For other crops, the residue removal factors in the USA were adopted from

Perlack et al. [2005]. For other countries with no data, removal factors were adopted from Krausmann et al. [2008],

who provide residue removal factors for major crop groupings and geographic regions.

Erosion, runoff and leaching of P

To estimate the P loads from diffuse sources, we followed the “surplus” approach of the Grey Water Footprint

Accounting Guidelines [Franke et al., 2013], in which the P load to fresh water is estimated by multiplying the surplus

P by an erosion-runoff-leaching fraction. The P surplus is estimated as P input of from mineral fertilizer and manure

minus the removal of P with harvested crops and crop residues. The erosion-runoff-leaching fraction (β) was estimated

as a function of the soil texture, soil erosion vulnerability, soil P content, rainfall intensity and management practices:

𝛽 = 𝛽JST U∑ 2V×WVV∑ WVV

X (𝛽J1# − 𝛽JST) (6)

The erosion-runoff-leaching fraction (β) will lie somewhere in between a minimum (βmin) and maximum (βmax),

depending on a number of environmental factors and management practice (Table S1). Per factor, the score for the

erosion-runoff-leaching potential (si) is multiplied by the weight of the factor (wi). We adopted the minimum

(βmin=0.0001) and maximum (βmax=0.1) fractions, the scores per factor, and the weights of the factors provided by the

Grey Water Footprint Accounting Guidelines [Franke et al., 2013]. Soil parameters were obtained from ISRIC-WISE

[Batjes, 2012]. The soil erosion vulnerability map was obtained from from USDA [USDA, 2014b]. The soil P content

was obtained from Yang et al. [2013]. The precipitation data for the period 2002-2010 were obtained from the Climate

Research Unit of the University of East Anglia [Mitchell and Jones, 2005]. We have used the average annual

precipitation.

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Table S1. Factors influencing the erosion-runoff-leaching potential of P

Factor

Erosion-runoff-leaching potential

Very low Low High Very high Remark

Score (s) 0 0.33 0.67 1.0 Weight (w, %)

Soil texture 25 Sand Loam Silt Clay

Soil erosion vulnerability

25 Low Moderate High Very high The erosion vulnerability

data is given as low, moderate, high, and very high erosion vulnerability

Soil P content (g P/m2)

20 < 200 200 - 400 400 - 700 > 700

Rain intensity (mm/y)

15 Light (< 200 mm/y)

Moderate (200-500 mm/y)

Strong (500-2000

mm/y)

Heavy (>2000 mm/y)

Used annual average rain intensity

Management practice

15 Best Good Average Worst Assumed average

management practice Source: Franke et al. [2013]

Note: with exception of the “management practice” for all factors we have used spatial data as indicated in Table S2.

Text S1.2 Point sources of phosphorus

Domestic P loads

The P load from the domestic sector is estimated following Van Drecht et al. [2009]:

𝑃72W = (𝑃7@J + 𝑃[\": + 𝑃]\":) × 𝐷 × (1 − 𝑅_) + 𝑃7@J(1 − 𝐷) × 𝑓2W (7)

where Phsw is the P load from households to surface water (kg/person/y), Phum the human P emission (kg/person/y), D

the fraction of the total population that is connected to public sewerage systems (dimensionless), PLdet the P emission

from laundry detergent (kg/person/y), PDdet the P emission from dishwasher detergents (kg/person/y), fsw the fraction

of non-sewered human P which is discharged to surface water, and RP the overall removal of P through wastewater

treatment (dimensionless). The regional average values for the year 2000 of P emission related to detergent use (PLdet

and PDdet) were taken from Van Drecht et al. [2009]. The first part of the equation refers to the population connected

to sewerage systems and the second part to the population not connected to sewerage systems.

Human P emissions

Human P emissions are estimated based on dietary per capita protein consumption per country over the period from

2002 to 2010, from FAOSTAT [FAO, 2012a]. The P intake was estimated from the N intake based on an N:P ration

of 10:1 (on mass basis) [Sette et al., 2011; USDA, 2014a]. The N intake in the food is estimated by assuming an

average 16% N content in dietary per capita protein consumption [Block and Bolling, 1946; FAO, 2003]. About 97%

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of the P intake is assumed to be excreted in the form of urine and faeces and the remainder 3% of P intake is lost via

sweat, skin, hair, blood and miscellaneous [Calloway et al., 1971; FAO et al., 1985; Morée et al., 2013].

Data on connection to public sewerage system (D) were collected mainly from UN Statistics Division [UNSD, 2014],

for European countries from Eurostat [European Commission, 2014], and for OECD countries from OECD [OECD,

2014]. For other countries with no data on D, we used the regional average values from Van Drecht et al. [2009].

To estimate the P removal through wastewater treatment (RP), we distinguished three wastewater treatment types with

differing P removal efficiencies based on the work of Van Drecht et al. [2009]: primary treatment (10% P removal),

secondary treatment (45% P removal), and tertiary treatment (90% P removal). Data on the distribution of the different

treatment types for European countries were obtained from Eurostat [European Commission, 2014] and for OECD

countries from OECD [OECD, 2014]. For other countries, we adopted regional average values from Van Drecht et al.

[2009] .

Part of the P emissions from populations that are not connected to sewerage systems is recycled in agriculture

[Drechsel and Kunze, 2001], and another part is lost by leakage and seepage to soils and groundwater [Held et al.,

2006; Marshall, 2005]. Van Drecht et al. [2009] assume that part of the non-sewered human P will not enter the

surface water. However, we have assumed that the fraction of non-sewered human P, which is not recycled in

agriculture and not lost by leakage to soils and groundwater, discharged to surface water (fsw) is 10%. Given that data

suggest that in many parts of the world, human excreta may be discharged directly to surface water, the 10% may not

be unrealistic.

Industrial P load

Industries responsible for nutrient loads include the food, textile, paper & cardboard, grease & oil, tannery, and soap

industries [Billen et al., 1999]. Since there is a lack of data on industrial loads per sector, we have estimated the P load

from the industrial sector as a whole as a function of the emission from the gross human urban nutrient load. The ratio

of P loads from industrial to urban domestic ranges from 0.13 to 0.21 [Billen et al., 1999; Brion et al., 2008; Luu et

al., 2012; Quynh et al., 2005]. We have assumed an average value of 0.15. We further assumed that about 30% of the

total P load is lost in wastewater stabilization ponds following the works of Morée et al. [2013] and Billen et al. [1999].

Therefore, the P load from the industrial sector as function of the load of urban human households is:

𝑃S2W = 0.15 × 0.7 × [(𝑃7@J + 𝑃[\": + 𝑃]\":) × 𝑈 × (1 − 𝑅_)] (8)

where Pisw is the P load from industries to surface water (kg/person/y) and U fraction of the total population living in

urban areas (taken from FAO [2012a]).

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The P load from households and industries were plotted at 5×5 arc-minute resolution by combining the P loads in

kg/person/y per country with the population density (person/km2) obtained from CIESIN and CIAT [2005].

Table S2 summarizes the data sources and spatial resolution of the data used in this study.

Table S2. Summary of data sources

Data Source Resolution

Fertilizer application rate (kg/ha) IFA et al. [2002] ; FAO [2012b] ; Heffer [2009]

Country

Total P fertilizer consumption (kg/y) FAO [2012a] Country

Crop distribution (ha/y) Monfreda et al. [2008] At 5x5 arc-minute

Manure excretion rates (kg P/animal) Sheldrick et al. [2003] global average

Livestock density per animal category and production system (head/ha)

FAO [2012c] At 3x3 arc-minute

Slaughter weight per animal category (kg/head)

Mekonnen and Hoekstra [2010b] Per country and per production system

Fractions of manure that are produced during grazing and the fractions of manure that are not available for spreading on crop- and grasslands

Bouwman et al. [2013] Global average

Manure applied on cropland and grassland

Menzi [2002] ; Kellogg et al. [2000]; Bouwman et al. [2009; 2013]

Country and regional average

Average P content of irrigation water Lesschen et al. [2007] Global average

The irrigation application rate Mekonnen and Hoekstra [2010a] At 5x5 arc-minute

Crop yield Mekonnen and Hoekstra [2010a; 2011] At 5x5 arc-minute

P contents of crops and crop residues IPNI [2012]; FAO [2004]; Roy et al. [2006]; FAO [2004]

Global average values

Residue-to-product ration Eisentraut [2010] Global average values

Crop residue removal factors FAO [2004]; Ravindranath et al. [2005]; Graham et al. [2007]; Nelson et al. [2002]; Perlack et al. [2005]; Krausmann et al. [2008]

Country level, sub-national, regional

Minimum and maximum leaching-runoff fractions

Grey Water Footprint Accounting Guidelines [Franke et al., 2013]

Global average

Score for the leaching-runoff potential Grey Water Footprint Accounting Guidelines [Franke et al., 2013]

Global average

Weight of the factor Grey Water Footprint Accounting Guidelines [Franke et al., 2013]

Global average

Soil parameters ISRIC-WISE [Batjes, 2012] 5x5 arc-minute

Soil erosion vulnerability USDA [2014b] 30x30 arc-minute

Soil phosphorus content Yang et al. [2014] 30x30 arc-minute

Precipitation data Climate Research Unit of the University of East Anglia [Mitchell and Jones, 2005]

30x30 arc-minute

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Dietary per capita protein consumption FAOSTAT [FAO, 2012a] Country

Connection to public sewerage system UN Statistics Division [UNSD, 2014]; Eurostat [European Commission, 2014]; OECD [2014]; Van Drecht et al. [2009]

Country, regional average

Distribution of the different treatment types

Eurostat [European Commission, 2014]; OECD [2014]; Van Drecht et al. [2009]

Country, regional average

P emission related to detergent use Van Drecht et al. [2009] Regional average

Population density CIESIN and CIAT [2005] 30x30 arc-second

Fraction of the total population living in urban areas

FAO [2012a] Country

The P load from diffuse sources was estimated for 126 crops separately. But for the presentation, the crops were grouped as shown in Table S3.

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Table S3. Primary crops grouping

Crop code Crop (FAOSTAT) crop grouping Crop code Crop (FAOSTAT) crop grouping

15 Wheat

Cereals

358 Cabbages

Vegetables

27 Rice, Paddy 366 Artichokes 44 Barley 367 Asparagus 56 Maize 372 Lettuce 71 Rye 373 Spinach 75 Oats 388 Tomatoes 79 Millet 393 Cauliflower 83 Sorghum 394 Pumpkins, Squash, Gourds 89 Buckwheat 397 Cucumbers and Gherkins 97 Triticale 399 Eggplants 103 Mixed Grain 401 Chillies & Peppers, Green 108 Cereals nes 402 Onions + Shallots, Green 116 Potatoes

Roots

403 Onions, Dry 122 Sweet Potatoes 406 Garlic 125 Cassava 414 Beans, Green 136 Taro (Coco Yam) 417 Peas, Green 137 Yams 423 String Beans 149 Roots and Tubers nes 426 Carrots 236 Soybeans

Oil crops

430 Okra 242 Groundnuts in Shell 446 Green Corn (Maize) 249 Coconuts 463 Vegetables Fresh nes 254 Oil Palm Fruit 567 Watermelons 260 Olives 568 Cantaloupes & other Melons 265 Castor Beans 176 Beans, Dry

Pulses

267 Sunflower Seed 181 Broad Beans, Dry 270 Rapeseed 187 Peas, Dry 280 Safflower Seed 191 Chick-Peas 289 Sesame Seed 195 Cow Peas, Dry 292 Mustard Seed 197 Pigeon Peas 299 Melonseed 201 Lentils 328 Seed Cotton 205 Vetches 333 Linseed 210 Lupins 339 Oilseeds nes 211 Pulses nes 156 Sugar Cane Sugar crops 157 Sugar Beets

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Crop code Crop (FAOSTAT) crop grouping Crop code Crop (FAOSTAT) crop grouping

217 Cashew Nuts

Nuts

486 Bananas

Fruits

220 Chestnuts 489 Plantains 221 Almonds 490 Oranges 222 Walnuts 495 Tang.Mand.Clement.Satsma 223 Pistachios 497 Lemons and Limes 225 Hazelnuts (Filberts) 507 Grapefruit and Pomelos 234 Nuts nes 512 Citrus Fruit nes 656 Coffee, Green

Other crops

515 Apples 661 Cocoa Beans 521 Pears 667 Tea 526 Apricots 677 Hops 530 Sour Cherries

687 Pepper, White/Long/Black 531 Cherries

689 Pimento, Allspice 534 Peaches and Nectarines 692 Vanilla 536 Plums

702 Nutmeg, Mace,

Cardamons 541 Stone Fruit nes, Fresh 711 Anise, Badian, Fennel 544 Strawberries 720 Ginger 547 Raspberries 723 Spices nes 549 Gooseberries 773 Flax Fibre and Tow 550 Currants 780 Jute 552 Blueberries 782 Jute-Like Fibres 554 Cranberries 789 Sisal 558 Berries nes 821 Fibre Crops nes 560 Grapes 826 Tobacco Leaves 569 Figs 836 Natural Rubber 571 Mangoes Fodder crops 572 Avocados

574 Pineapples 577 Dates 592 Kiwi Fruit 600 Papayas 603 Fruit Tropical Fresh nes 619 Fruit Fresh nes

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Text S2: Additional results

Table S4 presents the annual global P inputs from mineral fertilizer and manure, P removal with harvested crops and crop residues removed, and P erosion, runoff and leaching to fresh water systems per crop category. The P load from diffuse source has increased from 525 Gg in 2002 to 666 Gg in 2010 (a 27% increase). This increase is due mainly to the increase in P from the mineral fertilizer that has increased by 31% from 2002 to 2010.

Table S4. Global annual P inputs from mineral fertilizer and manure, P removal with crop and crop residues, and P erosion, runoff and leaching to freshwater systems per crop category (Gg/y)

Crop/ components in P balance 2002 2003 2004 2005 2006 2007 2008 2009 2010 Average

P in mineral fertilizer Cereals 8202 8486 9338 9603 9787 9702 8540 9746 11115 9391

Fruits 658 698 772 794 803 783 657 729 917 757

Vegetables 876 913 1061 1139 1136 1014 879 1019 1176 1024

Oil crops 2440 2736 3138 2957 2973 2918 2561 2729 3278 2859

Pulses 256 258 262 273 255 246 193 211 255 245

Roots & tubers 520 539 590 595 573 554 477 513 620 553

Sugar crops 493 535 553 512 545 616 523 526 616 546

Nuts 104 112 133 131 138 134 108 118 140 124

Other crops 1444 1491 1493 1494 1506 1511 1461 1525 1570 1500

Total P in mineral fertilizer 14992 15768 17340 17498 17718 17477 15400 17116 19687 17000 P in mineral manure Cereals 868 883 874 849 857 876 878 881 884 872

Fruits 1505 1529 1523 1495 1515 1540 1544 1555 1560 1530

Vegetables 1167 1182 1175 1155 1170 1189 1192 1199 1202 1181

Oil crops 641 651 647 636 644 653 660 667 672 652

Pulses 576 587 584 569 576 590 589 591 591 583

Roots & tubers 204 207 207 206 210 211 213 216 218 210

Sugar crops 124 126 126 124 125 127 128 128 129 126

Nuts 220 222 223 223 227 228 229 233 233 227

Other crops 500 506 505 502 508 512 520 527 533 513

Total P in manure 5806 5893 5865 5758 5832 5926 5953 5997 6022 5895 P removed with crop and crop residues Cereals 7019 7232 7850 7825 7716 8105 8708 8578 8337 7930

Fruits 195 201 213 216 224 225 232 237 241 220

Vegetables 168 175 175 181 189 196 203 206 198 188

Oil crops 2106 2251 2461 2580 2625 2695 2749 2639 2938 2561

Pulses 283 289 289 295 297 301 306 310 332 300

Roots & tubers 166 165 173 171 163 165 171 170 169 168

Sugar crops 154 152 152 151 160 175 180 175 177 164

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Crop/ components in P balance 2002 2003 2004 2005 2006 2007 2008 2009 2010 Average

Nuts 2.58 2.66 2.72 3.08 3.32 3.50 3.93 3.79 3.93 3.28

Other crops 1289 1289 1298 1298 1304 1304 1308 1307 1309 1301 Total P removed with crop and crop residues 11384 11758 12615 12720 12680 13170 13862 13626 13704 12835 P erosion, runoff and leaching from anthropogenic sources Cereals 156 161 175 191 209 182 79 158 253 174

Fruits 79.3 81.7 84.0 83.6 84.5 84.6 79.4 82.6 90.1 83.3

Vegetables 76.9 78.7 84.5 86.7 86.9 82.3 76.7 82.5 89.4 82.7

Oil crops 82.9 95.1 109.4 86.3 84.8 76.2 46.3 67.3 86.6 81.7

Pulses 28.3 28.6 28.7 28.2 27.6 27.6 24.6 25.5 26.5 27.3

Roots & tubers 24.6 25.6 27.5 27.7 27.3 26.4 23.0 24.6 29.4 26.2

Sugar crops 18.8 20.6 21.3 19.7 20.7 23.0 19.2 19.5 23.0 20.7

Nuts 13.5 13.9 14.8 14.7 15.2 15.0 14.0 14.6 15.5 14.6

Other crops 45.0 47.8 47.6 47.5 48.1 48.3 45.8 49.6 52.4 48.0 P erosion, runoff &leaching from anthropogenic sources 525 554 593 585 604 566 408 524 666 558

The annual P load from point sources and the global total annual GWF per sector are presented in Table S5 and S6, respectively. The global GWF has increased by about 15% within the study period, with the agricultural sector showing the largest growth (by 27% from 2002 to 2010). The contribution of the diffuse sources to the total GWF has grown from 37% in 2002 to 41% in 2010, while that of domestic sector dropped from 55% in 2002 to 51% in 2010.

Table S5. P loads from domestic and industrial sources (Gg/y), per year.

2002 2003 2004 2005 2006 2007 2008 2009 2010 Average Domestic 769 776 783 791 798 806 814 822 830 799 Industry 111 112 114 115 116 117 118 120 121 116 Total 880 888 897 905 914 923 932 941 951 915

Table S6. Total GWF related to P loads to fresh water (1012 m3/y), per year.

Sectors 2002 2003 2004 2005 2006 2007 2008 2009 2010 Average Agriculture 52.5 55.4 59.3 58.5 60.4 56.6 40.8 52.4 66.6 55.8 Domestic 76.9 77.6 78.3 79.1 79.8 80.6 81.4 82.2 83.0 79.9 Industry 11.1 11.2 11.4 11.5 11.6 11.7 11.8 12.0 12.1 11.6 Total 141 144 149 149 152 149 134 147 162 147